Accepted Manuscript

A critical review on remediation, reuse, and resource recovery from acid mine
drainage

Gayathri Naidu, Seongchul Ryu, Ramesh Thiruvenkatachari, Youngkwon Choi,

Sanghyun Jeong, Saravanamuthu Vigneswaran

PII: S0269-7491(18)35255-2
DOI: https://doi.org/10.1016/j.envpol.2019.01.085
Reference: ENPO 12124

To appear in: Environmental Pollution

Received Date: 22 November 2018

Revised Date: 6 January 2019
Accepted Date: 17 January 2019

Please cite this article as: Naidu, G., Ryu, S., Thiruvenkatachari, R., Choi, Y., Jeong, S., Vigneswaran,
S., A critical review on remediation, reuse, and resource recovery from acid mine drainage,
Environmental Pollution (2019), doi: https://doi.org/10.1016/j.envpol.2019.01.085.

This is a PDF file of an unedited manuscript that has been accepted for publication. As a service to
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 ACCEPTED MANUSCRIPT
Graphic Abstract

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1 A Critical Review on Remediation, Reuse, and Resource Recovery from Acid

2 Mine Drainage

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4 Gayathri Naidua, Seongchul Ryua, Ramesh Thiruvenkatacharib, Youngkwon Choia, Sanghyun

Jeongc, Saravanamuthu Vigneswarana,*

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a
7 Faculty of Engineering, University of Technology Sydney (UTS), P.O. Box 123, Broadway NSW 2007, Australia

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8 Commonwealth Scientific and Industrial Research Organisation (CSIRO), 1 Technology Court, Pullenvale, Queensland 4069,

9 Australia
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10 Graduate School of Water Resources, Sungkyunkwan University (SKKU), 2066 Seobu-ro, Jangan-gu, Suwon-si, Gyeonggi-do

11 16419, Republic of Korea

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13 *Corresponding author: Tel +61-2-9514-2641; Fax +61-2-9514-2633; Email: Saravanamuth.Vigneswaran@uts.edu.au
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15 Abstract

16 Acid mine drainage (AMD) is a global environmental issue. Conventionally, a number of active
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17 and passive remediation approaches are applied to treat and manage AMD. Case studies on

18 remediation approaches applied in actual mining sites such as lime neutralization,

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19 bioremediation, wetlands and permeable reactive barriers provide an outlook on actual long-term
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20 implications of AMD remediation. Hence, in spite of available remediation approaches, AMD

21 treatment remains a challenge. The need for sustainable AMD treatment approaches has led to

22 much focus on water reuse and resource recovery. This review underscores (i) characteristics and

23 implication of AMD, (ii) remediation approaches in mining sites, (iii) alternative treatment

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24 technologies for water reuse, and (iv) resource recovery. Specifically, the role of membrane

25 processes and alternative treatment technologies to produce water for reuse from AMD is

26 highlighted. Although membrane processes are favourable for water reuse, they cannot achieve

27 resource recovery, specifically selective valuable metal recovery. The approach of integrated

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28 membrane and conventional treatment processes are especially promising for attaining both

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29 water reuse and recovery of resources such as sulfuric acid, metals and rare earth elements.

30 Overall, this review provides insights in establishing reuse and resource recovery as the holistic

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31 approach towards sustainable AMD treatment. Finally, integrated technologies that deserve in

32 depth future exploration is highlighted.

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34 Keywords: Acid mine drainage; membrane processes; rare earth elements; resource recovery;

water reuse
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37 Capsule
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38 Challenges associated with AMD can be sustainability addressed through integrated treatment

39 approaches that attain both water reuse and valuable resource recovery
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40

41
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42 1. Introduction
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43 Acid mine drainage (AMD) is a challenge encountered by mining industries globally. AMD

44 primarily results from the oxidation of pyrite as well as other sulfate metals upon exposure of

45 mining sources to air, microbial activities and water (Dold, 2008). These mining sources include

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46 ore and rock waste piles, open exposed cuts and tailing pits and dams, mines underground, as

47 well as sulfuric acid soils (DIIS, 2016).

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49 The general features of AMD (also sometimes referred to as acid rock drainage or acidic-metallic

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50 drainage) are extreme acidity with elevated concentration of sulfate and metals (primarily iron,

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51 aluminum, and zinc, and other heavy metals). Invariably, the release of untreated AMD poses a

52 risk of contaminating nearby water sources and sediments with detrimental effect on biodiversity

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53 (Winterbourn et al., 2000). Nevertheless, an accurate assessment of the economic scale and

54 environmental liability caused by AMD remains challenging.

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56 Some of the major global mining operations are located in Canada, Australia, the United States,

and South Africa (Hilson, 2002). According to the United States (US) Forest Service, in 2010,
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58 more than 6,000 km of streams are projected to be polluted due to AMD from coal mines in
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59 eastern US. Meanwhile in western half of the country, forest lands are exposed to acid discharges
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60 from around 20,000 to 50,000 mines, impacting a substantial amount of streams (between 8,000 -

61 16,000 km streams) (Easton, 2018, USDA, 1993, Ziemkiewicz et al., 2003). The cost of AMD
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62 remediation at abandoned mines in North America alone is estimated to be approximately $10

63 billion. The Canadian Mine Environment Neutral Drainage Program estimates that total
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64 environmental liability costs due to AMD at mine sites could be approximately CAD 2 to 5
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65 billion (MEND, 2001). In South Africa, AMD contribution has been attributed to the presence of

66 significantly large amount of abandoned mine sites and huge pyrite-bearing tailings from coal

67 and gold mines in Witwatersrand basin (Mhlongo and Amponsah-Dacosta, 2016).

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69 Australia is among the world’s top producers for many important minerals; in 2015, the

70 country’s mineral exports (apart from petroleum goods) was around AUD141 billion,

71 approximately 9% of its gross domestic product (Britt et al., 2016). There are currently about 380

72 mines in operation in Australia (Britt et al., 2017). Due to data limitations and ambiguity in the

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73 definition of abandoned mines, the exact number of abandoned mines in Australia is unknown;

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74 however, it is believed to be as high as several thousand (Venkateswarlu et al., 2016) as shown in

75 Fig. S1. An early analysis on mining activities in Australia reported that 317 out of 517 mines

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76 consist of waste materials with the possibility to generate acid (Harries, 1997). In Australia, acid

77 sulfate soils occur both inland and along coastlines, occupying approximately 215,000 km2 of

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total land area, with 58,000 km2 and 157,000 km2 identified along the coastline and inland
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79 respectively (Fig. S2) (Fitzpatrick et al., 2009).
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81 AMD produced from an operational mine can often be managed at a relatively lower cost than
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82 after closure. However, in Australia, from the early 1980s up to 2005, closure of approximately
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83 70% mining sites were unplanned due to aspects such as the low cost of supplies, costly

84 operations, reduced reserves, and challenging geotechnical settings (Laurence, 2006). Annual
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85 AMD management in Australia is estimated to be approximately $150 million for operating

86 mines and well over $500 million for abandoned mine sites (Harries, 1997).
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88 The environmental and economic impacts of AMD have spurred strategic development of cost-

89 effective prevention and remediation solutions (Kalin et al., 2006). Preventive strategies are ideal

90 as they preclude the formation of AMD at the source itself. Nevertheless, preventing AMD

91 generation is highly challenging in practical terms (Johnson and Hallberg, 2005). Active and

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92 passive remediation methods are currently considered the most practical option for treating AMD

93 (Johnson and Hallberg, 2005, Skousen et al., 2000). Although AMD remediation methods are

94 widely adopted at most mining sites today, the suitability and performance of these methods vary

95 depending on site-specific context such as geographical condition and weather (Johnson and

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96 Hallberg, 2005, RoyChowdhury et al., 2015). Conventional pH control with cost-effective

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97 neutralization reagents is the most widely used and least inexpensive approach for AMD

98 remediation treatments (Kalin et al., 2006, Taylor et al., 2005). Nevertheless, it results in sludge

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99 production that requires further management and appropriate disposal. For instance, an average

100 of 6.7 million cubic meters of sludge is estimated to be produced annually by AMD

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neutralization treatment process in Canada (Zinck, 2004, Zinck et al., 1996).
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Currently, the mining industry faces increasing pressure to embody principles of sustainable
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104 mining. This has resulted in a paradigm shift towards reducing the volume of sludge generated as
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105 well as the operating cost, and improving treatment efficiency. Arguably, a key element of
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106 sustainable mining is reuse of mining and mineral-processing waste (Macías et al., 2017,

107 Masindi, 2017). Although many researchers have discussed the aspect of metal precipitation
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108 from AMD (Johnson and Hallberg, 2005, Kalin et al., 2006, RoyChowdhury et al., 2015), only a

109 handful have focused on the recovery of valuable metals (Kefeni et al., 2017), sulfuric acid
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110 (Nleya et al., 2016), and water for reuse (Masindi, 2017). Further, the prospects of recovering
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111 rare earth elements from AMD is a promising possibility that could potentially offset AMD

112 treatment cost (Ayora et al., 2016). The key drivers for enabling water reuse and valuable

113 resource recovery are innovative treatment technologies such as membrane processes as well as

114 the integration of conventional and alternative processes. However, approaches for AMD reuse

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115 and resource recovery has not been assessed in detail. This review article intends to bridge this

116 gap (Fig. 1).

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118 Hence, the objective of this review article is to provide a better understanding of AMD treatment

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119 by discussing the varying characteristics of AMD and its environmental and economic impacts.

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120 Accordingly, this work describes case studies of AMD remediation methods applied at actual

121 mining sites and their challenges. Thereafter, the discussion accentuates to future perspectives

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122 for AMD treatment. Specifically, the aspect of innovative research using integrated processes for

123 attaining AMD reuse and resource recovery is explored in detail.

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125 Fig. 1. Holistic approach towards sustainable AMD treatment in the mining industry.
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127 2. Characteristics of AMD

128 AMD is primarily generated when the mineral pyrites (iron) are exposed to air, water and

129 microbial activity (Kalin et al., 2006, Taylor et al., 2005) (Fig. 2). Pyrites go through a dual stage

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130 oxidation process, firstly generating ferrous sulfur and sulfuric acid, and thereafter, ferric

131 hydroxide that is reddish orange with additional sulfuric acid. The chemical reaction of AMD

132 generation is a well-understood process and has been described in detail by many previous

133 studies (Akcil and Koldas, 2006, Johnson and Hallberg, 2005, Kalin et al., 2006, Simate and

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134 Ndlovu, 2014).

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136 The characteristics of AMD vary widely as the generation of AMD tend to rely on varying site

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137 conditions such as weather, geomorphology, and the amount of waste materials (Schaider et al.,

138 2014; Nieva et al., 2018). Chemical, biological, and physical factors that mainly influence the

139
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level of AMD generation includes air (oxygen), temperature such as rain and water saturation
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140 levels, microbial activity and degree of metal sulfide exposure (Akcil and Koldas, 2006) (Fig. 2).
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142 Fig. 2. AMD generation and related contamination pathway.

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144 Mine water characteristics from varied sampling locations such as operating and abandoned mine

145 sites, open pits, waste rock piles, mine shafts, downstream river and creeks have been widely

146 reported by previous studies (Table S1). Based on these data, the distribution characteristics of

147 AMD close to mining sites and downstream are depicted in Fig. 3. On average, water samples at

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148 mine sites close to AMD tend to be highly acidic with high concentrations of sulfate (1,000–

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149 130,000 mg/L) and dissolved ferrous metals (200–1,000 mg/L). The acidic condition increases

150 the solubility of major metals such as Zn and Al (20–800 mg/L) as well as other metals such as

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151 Cu, Mn, and Ni (trace concentrations to 250 mg/L). AMD tends to become increasingly

152 neutralized further downstream due to dilution coupled with reactions with river sediment.

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Nevertheless, certain constituents, such as sulfate and metals, have high solubility and remain in
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154 the water (Cozzolino et al., 2018; Migaszewski et al., 2018).
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157 Fig. 3. Distribution of metal ions as a function of pH of water samples collected near mining
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158 sites and from downstream rivers. The data were sourced from previous studies (Table S1).
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159 3. Implications of AMD

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160 3.1. Economic implications

161 AMD has a significant impact on the economics of a mining operation, especially for large
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162 mining sites. One of the largest locations of AMD in the United States is the Berkeley Pit located
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163 in Butte, Montana. The pit contains over 95 billion liters of AMD and covers an area of 1.7 km2.

164 The accumulation rate of water into the pit is approximately 11 million liters a day, resulting in a

165 rise in the water level of approximately 3 m every 9 months (Tabak et al., 2003). Similarly, Chen

166 et al. (2007) indicated that around 15,000 m3/day of AMD is produced from Liwu mud-retaining

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167 dam located in a mining region in northern Guangdong, China. The AMD contaminates soil and

168 various natural water sources located downstream from the mine.

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170 The combined cost of AMD treatment for four major mining countries in the world is estimated

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171 to range from USD 32–72 billion (Cozzolino et al., 2018). At an estimated treatment cost of

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172 CAD 2 to 5 billion (depending on the type of treatment and control technology used), AMD has

173 been identified as one of the largest liability facing the Canadian mining industry (MEND,

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174 2000). In Australia, mines are generally medium in size with open pits as well as underground

175 mines. In the case of open pit mines with large tailing features, the operating cost can exceed

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AUD 50 million. Moreover, AMD generation incurs an additional cost in regards to water
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177 treatment of water system and rehabilitation of waste (Cozzolino et al., 2018). The remediation

cost of treating AMD at abandoned mine sites is estimated to be higher than that at operating
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179 sites (Harries, 1997).

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181 3.2 Environmental implications

182 The significant long-term environmental impact of AMD (Fig. 2) is mainly due to pH reduction
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183 as well as enhanced contents of heavy metal in close by streams and soils. AMD has a tendency

184 to infiltrate aquifers as well as generate effluents that converge into water streams, polluting
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185 fresh water sources (Fig. S3). The impact of AMD contamination on the ecology of streams and
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186 aquatic organisms such as fish has been widely established by previous studies (Akcil and

187 Koldas, 2006, Simate and Ndlovu, 2014, Taylor et al., 2005). Studies have also implicated the

188 long term mining effect and contaminated soils towards plant growth and human health owing to

189 metals leaching from the soil (Neamtiu et al., 2017; Bonnail et al., 2018).

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190

191 4. Prevention

192 Prevention refers to the inhibition of AMD formation at the point of its original generation,

193 limiting sulfide waste exposure to air, rain (water sources) and sulfide reducing bacteria (Kefeni

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194 et al., 2017, Michel Aubertin et al., 2016). Prevention is an ideal solution as it permanently

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195 precludes the formation of AMD and hence requires no further management such as sludge

196 disposal (Diao et al., 2013, Sánchez-Andrea et al., 2014). Prevention of AMD formation mainly

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197 requires protection of sulfide minerals from air, water, and bacteria. This can be done by several

198 approaches that use clay, soil, geotextiles, plant cover or any other limiting agent, and which

199
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200 of various AMD prevention approaches and their limitations are listed in Table S2.
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202 Notably, preventive approaches are practically difficult to implement and the next available
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203 option—and often the last resort—is to adopt remediation methods to minimize the impact of
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204 AMD pollution on wider environments such as receiving streams and rivers. The various AMD

205 remediation approaches are discussed in the following section.

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207 5. Remediation

208 AMD can present a substantial risk of incurring significant costs if it is not identified early and

209 managed appropriately. In order to attain sustainable mining rehabilitation, managing the

210 environmental aspects throughout the duration of the active mining operation is critical.

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211

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212 The central Australian Government in consultation with its state and territory counterparts has

213 established a Land Access for Resources Working Group (LARWG) for the management of

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214 abandoned mines by emulating best practice scenarios and to implement the recommendations

215 from the strategic framework (Pepper et al., 2014). Other countries, such as Canada, have also

216
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introduced various initiatives to manage abandoned mines and AMD, such as the National
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217 Orphaned and Abandoned Mine Initiative (NAOMI, 2015, Tremblay and Hogan, 2012).
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219 AMD remediation can be broadly classified as active and passive treatment approaches. Active
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220 treatment methods commonly involve the usage of a variety of neutralizing agents to ensure the
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221 effluent meet the required discharge standard. A broad range of active treatment approaches for

222 AMD remediation are available. The main chemical and physical processes of active treatment
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223 (in-site and fixed plant) include precipitation (pH control and electrochemical process), sulfate

224 reduction through biological/microbial mediation, flocculation, adsorption and ion exchangers,
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225 filtration, as well crystallization (Brown et al., 2002).

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227 By far, the most common and generally adopted active primary treatment is chemical

228 neutralization (Taylor et al., 2005). In large scale AMD treatment, commonly utilized

229 neutralizing agents include caustic soda (sodium hydroxide), lime and limestone, magnesium

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230 oxide and hydroxides. Amongst these neutralizing agents, limestone is vastly used due to its low

231 cost. Nevertheless, neutralization and precipitation through pH change alone is not sufficient,

232 especially when metals such as arsenic, molybdenum, mercury, selenium and chromium are

233 present. A secondary stage of treatment is therefore necessary. Moreover, another challenge of

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234 neutralization approach is the production of aqueous sludge (more than 90% water) containing

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235 heavy metals. Dewatering the sludge incurs additional cost.

236

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237 In terms of AMD remediation, active treatments are generally considered expensive compared to

238 passive treatment, especially when the mining operation has ceased (Santos Jallath et al., 2018).

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Passive treatment methods generally achieve precipitation of metal sulfide by creating reducing
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240 conditions and utilizing organic substances as alkaline agents. Minimal or periodic maintenance

and inspection is one of the main difference of passive treatment over active treatment (Taylor et
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242 al., 2005). Passive treatment methods include aerobic wetlands, compost reactors, anoxic and
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243 open limestone drains and channels, bioreactors, permeable reactive barriers.
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245 Passive treatment application can be economically attractive in scenarios of low acid loads with
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246 minimal water flow rate fluctuations. They are not unsuitable for conditions exceeding 150 kg

247 CaCO3 per day (Taylor et al., 2005). For instance, wetland is an attractive low cost passive
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248 treatment approach that can potentially achieve better effluent quality compared to active
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249 neutralizing treatment. Nevertheless, wetland applications are restricted to AMD with near

250 neural and low acidic characteristics (pH exceeds 4.5) and cannot handle and adjust to rapid

251 changes in water quality and flow rates (Caraballo et al., 2011). Hence, in order for passive

252 treatments such as wetlands to be effectively implemented, prior specialist knowledge of the

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253 physical and chemical behavior of situ treatment ponds or pits containing AMD must be carried

254 out. Moreover, although passive treatment require minimal maintenance, eventual renovation is

255 the norm which incurs additional cost (Skousen et al., 2017). Further, toxic metal accumulation

256 and its related long-term effect must be carefully addressed.

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257

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258 Detailed descriptions of various active and passive remediation methods have been reported by

259 previous studies (Akcil and Koldas, 2006, Johnson and Hallberg, 2005, Kefeni et al., 2017,

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260 Moodley et al., 2017, RoyChowdhury et al., 2015, Simate and Ndlovu, 2014). The practical

261 implementation and performance capacity of both active and passive AMD remediation

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treatments have resulted in the wide adoption of these approaches at mining sites. However, only
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263 limited studies have discussed this aspect (Akcil and Koldas, 2006, Gibert et al., 2011). A few

case studies on remediation treatment application at actual mining sites are briefly discussed
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265 here.
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267 5.1 Case studies of remediation method at actual mining site: High-density sludge (Iron

268 Mountain Mine, California, United States)

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269 A widely adopted method for AMD treatment is lime neutralization, which not only neutralizes

270 acid but also precipitates metals as oxides/hydroxides. High-density sludge (HDS) treatment is a
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271 more refined method of aeration and sludge recycling. HDS effectively recycles sludge to utilize
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272 more lime and to apply efficient flocculation processes to produce dense sludge with up to 30%

273 or more solids. Due to these advantages, HDS treatment for AMD management has been adopted

274 at several mining operations around the world. One such case study is discussed here.

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276 Iron Mountain Mine site, located in Shasta County, California, was used for mining mainly iron

277 as well as copper, gold, silver, zinc and pyrite from the 1860s through 1963. The site covers an

278 area of 16,200 m2 (ITRC, 2010). Although not in operation any longer, the mining site still

279 contains mine tailings and waste rocks, open and underground mine pits and workings. Reports

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280 highlighted that the AMD contained at these sites are highly acidic (measured pH values being

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281 lower than 1), and the concentrations of metal and sulfate in combination can range between 200

282 g/L up to 760 g/L. Heavy metals, mainly copper, zinc, cadmium leaches out as the acid flow out

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283 through the mountain sites into creeks. Ultimately, a substantial amount of the AMD flows into

284 the Spring Creek Reservoir. From 1994 to 1996, a full-scale HDS neutralization system was

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installed and operated at the Iron Mountain mine site (Fig. S4). The remediation approach via
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286 HDS neutralization successfully reduced acid as well as contaminated heavy metals in the water

streams. However, at an estimated total capital cost of $200 million, the treatment was
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288 expensive, and operation and maintenance costs amounted to $5–6 million per year. Apart from
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289 the cost, the disposal area for sludge is expected to reach its full capacity by the year 2030,
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290 invariably requiring new and improved remedial approaches.

291
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292 5.2 Case studies of remediation method at actual mining site: Successive alkalinity-

293 producing systems (Hanchang Coal Mine of Kangwon, Korea)

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294 Successive alkalinity-producing systems (SAPS) offer alternative treatment for AMD and
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295 involves bioremediation (Nairn and Mercer, 2000). SAPS comprises of passing AMD vertically

296 through a layer of substrate overlying a limestone bed. This is a commonly used passive

297 treatment approach, and one such case study is discussed here.

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299 A passive SAPS treatment approach was constructed in June 2001 at Hanchang Coal Mine,

300 Kangwon, Korea (Fig. S5) (CIPB, 2004) to treat AMD at a rate of 300 m3 per day. The SAPS

301 neutralization treatment functions by vertically channeling AMD through limestone beds.

302 Organic substrates (spent mushroom compost) were placed over the limestone beds. Investment

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303 in design and construction was expected to minimize acidity and sulfate concentrations for five

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304 years. Contrarily, a performance assessment revealed that within the first year of the treatment,

305 sulfate reduction in the vertical flow reactor was ineffective (Bhattacharya et al., 2008). This was

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306 attributed to adsorption and precipitation of the metal hydroxides, which superseded the

307 precipitation and formation of sulfide based metals. Moreover, fluctuation in the SAPS loadings

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due to seasonal and heavy flooding affected the performance of the compost substrate. One of
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309 the promising features of SAPS is sulfate reduction through bacterial activity from the compost

substrate. However, the performance assessment reported on the minimal reduction in sulfate
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311 contents through bacterial activity. As a results of this, sulfate concentration in the effluent
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312 increased due to leaching through the compost substrate.

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314 The effective application of SAPS treatment design is highly dependent on geochemical
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315 conditions. Changes in loading due to natural weather circumstances greatly affect SAPS

316 performance. Therefore, the same design concept is not applicable to all mining sites. Further,
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317 the system requires ongoing maintenance, which incurs additional costs.
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319 5.3 Case studies of remediation method at actual mining site: Wetlands (Beacon Compost

320 Wetland, Australia)

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321 Wetlands are a promising passive treatment option as they are relatively self-sustaining once

322 established and are deemed to be cost effective (Akcil and Koldas, 2006, Johnson and Hallberg,

323 2005, RoyChowdhury et al., 2015, Taylor et al., 2005). A case study of a wetland in Australia is

324 discussed here.

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325

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326 The Beacon compost wetland is a shallow treatment cell (100 m long × 3 m wide × 1 m deep)

327 utilizing composted sheep manure (Fig. S6) (Degens, 2009). A report on the performance

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328 monitoring of the wetland noted that it attained maximum AMD treatment within the first 100-

329 124 days. Thereafter, the treatment efficiency decreased. Reduced treatment rates were attributed

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to inconsistent and shallow flows and pond water in the course of seasonal change (summer to
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331 autumn). These factors enhanced oxidizing conditions of the wetland, reducing the treatment

effectiveness. In warmer seasons (summer to autumn), enhanced rate of decomposition is

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333 anticipated. However, the influence of oxidation on the organic matter underlay as well as in the
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334 surface water was associated with the inability of the wetland to sustain conducive settings suited
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335 for biological sulfate reduction.

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337 Similarly, in other cases (Akcil and Koldas, 2006, Eger and Wagner, 2002, Groudev and

338 Komnitsas, 2003), the efficiency of wetlands for AMD treatment has been established in
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339 controlled scenarios only. For instance, rapid changes in the concentration and flow rate as well
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340 as oxidation and precipitation are aspects that significantly hinder the performance of wetlands

341 for AMD remediation. Further, geographical conditions such as large land requirement as well as

342 slopes that are not steep and soils without rocks are necessary for the application of wetlands.

343 Weather conditions such as flood and seasonal variations also restrict the usage of wetlands.

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344 5.4. Case studies of remediation method at actual mining site: Permeable reactive barrier

345 (Mt Carrington Silver and Gold Mine, northern New South Wales, Australia)

346 Permeable reactive barriers (PRBs) is an in-situ remediation approach containing reactive barrier

347 of materials that are buried to intercept AMD trails from groundwater (Scherer et al., 2000,

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348 Taylor et al., 2005). Reactive materials include zerovalent ions, organic matter as well as

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349 limestone. This treatment technology has shown great promise for AMD remediation (Gibert et

350 al., 2011, Shabalala et al., 2017).

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352 PRBs were tested as an AMD remediation approach at a silver and gold mining site at Mt

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Carrington, New South Wales, Australia (Munro et al., 2004, Thiruvenkatachari et al., 2008). For
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354 this test, the reactive material used was seawater-neutralized red-mud Bauxsol (a byproduct from

refining aluminum). Bauxsol was mixed with sand to overcome challenges of its inherent
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356 characteristics (fine-grained with low hydraulic conductivity). The PRB of Bauxsol with sand
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357 material was used to treat more than 45,000 L AMD above ground and achieved reduction in
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358 metal concentrations, in line with the Australian water quality standards. Further, clogging was

359 minimized by combining Bauxsol with sand as reactive materials for the PRB. Typical materials
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360 such as carbonates and hydroxides results in major clogging issues. Although efficient metal

361 removal rate was achieved, the spent Bauxsol requires safe disposal to landfills.
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363 PRBs are only effective for specific sites (AMD plumes must be less than 20 m below the

364 ground and only water with low concentration of oxygen can be in direct contact with the

365 reactive barrier). Therefore, mine sites must be well characterized and modeled prior to

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366 treatment. Further, PRB treatment needs multiple substrates to be effective, making the capital

367 and implementation cost high for large barriers (Gibert et al., 2011, Taylor et al., 2005).

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369 Overall, although remediation treatment does offer a practical solution to reduce AMD-

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370 associated environmental liabilities, these methods still suffer from significant limitations.

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371 Successful remediation treatment cannot be applied arbitrarily to each site. Suitable remediation

372 treatment highly depends on site-specific operation and installation, alongside with a

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373 combination of technologies suited to AMD chemical constituents and acidic load. Moreover,

374 most treatment approaches require maintenance and/or regular reagent addition as well as careful

375 sludge disposal.

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For instance, Zinck and Griffith (2013) indicated that, in over 100 operating mines around the
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378 world, an average of 9500 tonnes of dry sludge is produced annually from active and passive
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379 remediation. Globally, a higher increase in the amount of sludge produced is anticipated due to
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380 the increase in the activities of metal mines per the demand for metals and the implementation of

381 stricter environmental regulations (Macías et al., 2017).

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382 6. Sustainable mining practices

383 The motivation towards reducing waste sludge and brine has drawn much attention on

384 developing sustainable AMD treatment technologies. For instance, a recent study in

385 Pennsylvania (Wang et al., 2018) systematically carried out a quantitative comparison on the

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386 implication of direct release of AMD to the ecosystem over the energy implication of setting up a

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387 pilot scale co-treatment remediation process (combining produced water and AMD). The results

388 of this study demonstrated the greater magnitude of benefits in treating AMD sustainably such as

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389 a well-planned co-treatment process over the environmental implications of untreated AMD.

390 Water reuse is now acknowledged as a best practice due to its substantial advantages compared

391
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to the conventional remediation approach of treat and discharge. Moreover, AMD is increasingly
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392 recognized as a source of valuable resources, the recovery of which could generate revenue to

offset ongoing treatment costs, rather than just waste that needs to be treated and disposed. The
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393

394 following section focuses on assessing various approaches for AMD reuse, namely, conventional
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395 and alternative membrane processes as well as the recovery of sulfuric acid, metals, and potential
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396 recovery of rare earth elements (Fig. 4).

397
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398 Fig. 4. Reuse and recovery of resources from AMD.

399
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400

401 6.1 Reuse

402 6.1.1 Conventional membrane processes

403 In recent times, membrane technologies, namely reverse osmosis (RO) and nanofiltration (NF),

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404 have been increasingly viewed as promising AMD treatment options for reducing discharge

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405 while producing good quality water for reuse. This is especially reflected by the increase of RO

406 and NF processes adopted at actual mining sites as well as research on AMD treatment using

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407 these technologies (Table 2). For instance, Chesters et al. (2016) identified 363 mines with the

408 potential to use RO and NF, and highlighted that approximately 67 mining sites globally have

409
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adopted RO to treat AMD, mainly in Peru and Chile. Similarly, Bonnelye (2015) described the
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410 application of RO for treating AMD at the largest copper mining plant in Chile. Recent studies

established the capability of a pilot-scale NF systems to treat AMD and produce a treated water
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411

412 stream suitable for industrial reuse (Wadekar et al., 2017, Andalaf et al., 2018).
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413
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414 The advantages of treating AMD with RO and NF include the capacity to meet strict

415 environmental discharge standards, with high efficiency and ease of operation. Moreover, the
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416 low salinity of AMD is especially advantageous for applying energy-efficient low-pressure NF

417 and RO. Although both RO and NF show promising water reuse capacity from AMD, membrane
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418 fouling is inevitable, necessitating pretreatment (Table 1). Meschke et al. (2015) used ceramic
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419 compact rotating disc microfiltration as a pretreatment, which removed almost all the Fe from

420 AMD, to minimize membrane fouling prior to RO. Similarly, a number of other studies used

421 sand filtration, aeration, microfiltration (MF) and ultrafiltration (UF) membranes, and adsorbents

422 as AMD pretreatment techniques prior to NF and RO (Aguiar et al., 2018, Wadekar et al., 2017,

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423 Wadekar and Vidic, 2018). Pretreatment increases the pH of AMD and removes major ions such

424 as SO4, Fe, and Mn.

425

426 It must be acknowledged that low energy consumption and operational cost are the premise for a

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427 technology to be adopted widely in an industry. Low-pressure RO and NF meet the criteria of

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428 low-energy processes; however, the operation cost is still relatively high and entails an additional

429 cost owing to the need for pretreatment. Moreover, although NF and RO treatments meet the

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430 discharge standards, a concentrated AMD waste stream is produced at a water recovery rate of

431 50–70%, which requires further management. On this basis, alternative treatment technologies

432 offer some promising advantages for treating AMD.

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433

Table 1 AMD treatment with nanofiltration (NF) and reverse osmosis (RO)
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434

Description Ref.
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NF pilot scale system using two different membranes (NF270 and NF90, France) was used to treat Andalaf et
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and model the behaviour of AMD. High rejection for all ions (~100%) were achieved, however, al., 2018

upon 75% water recovery, fouling was observed.

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NF (ceramic and polymeric NF270 membranes, pressure: 35 bar) were used to treat AMD obtained Wadekar

from a site in Pennsylvania (pretreated with aeration and microfiltration). NF270 rejected > 96% of and Vidic,
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multivalent ions. Use of ceramic membrane resulted in 55–67% rejections. Fouling (mostly gypsum) 2018
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of membranes occurred at 75% water recovery.

NF (polymeric NF270 membrane, pressure: 10 bar) was used to treat AMD obtained from a gold Aguiar et

mine in Brazil (pretreated with ultrafiltration). The treatment resulted in recovered water with good al., 2018

quality (i.e., 13.3 mg/L Ca and 262.1 mg/L SO4). Membrane fouling resulted in significant flux

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decline at 60% water recovery.

A single-pass RO (operational setting details not available) was used to treat AMD obtained from a Masindi,

coal mine in South Africa (pretreated with oxygen furnace slag and lime/soda ash softening). The 2017

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integrated pretreatment, followed by RO, resulted in the treated effluent meeting drinking water

standards.

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NF (polymeric NF90 membrane, pressure: 10 bar) was used to treat AMD obtained from a site in Wadekar et

Pennsylvania (pretreated with aeration, sedimentation, bag filtration, and ultrafiltration) and resulted al., 2017

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in 99% ion rejection. The recovered water was suitable for industry reuse.

RO and NF (polymer NF90 membrane) at the same operating pressure (10 bar) were used to treat Andrade et

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AMD obtained from a gold mine in Brazil. At 40% recovery rate, both NF90 and RO achieved al., 2017
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similar rejection rates but NF achieved a 7-fold higher permeate flux. NF was indicated to be more

suitable for AMD treatment at an estimated cost of USD 0.83/m³.

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NF (tight pores polymeric TS80 membrane) achieved 99% ion rejection of AMD from a copper Mullett et

mine in Western Australia. This was attributed to the membrane iso-electric point being higher than al., 2014
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the feed pH. The approach resulted in 70% water recovery, enabling the site to simultaneously meet
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environmental discharge standards and maximize copper recovery.

NF (polymeric NF2540 membrane) was suitable for the treatment and concentration of metallic and Sierra et al.,
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semi-metallic contaminants of AMD generated from mercury mining in the north of Spain, even at 2013

low pH and moderate pressures (pressure: 10–20 bar).

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RO and NF (NF99) at the same operating pressure (20 bar) were used to treat actual and synthetic Al-Zoubi et
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AMD. RO achieved higher rejections compared to NF but the latter was indicated to be more al., 2010

favorable as it achieved higher permeate flux.

NF system (polymeric NF99 membrane, pressure: 20 bar) was used to treat AMD from a Chilean Rieger et

copper mine. The results showed high rejection of toxic metals and sulfate, and met the al., 2009

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environmental discharge standards.

RO and NF (polymeric DK4040F membrane) at the same operating pressure (9–10 bar) was used to Zhong et

treat AMD from Dong Gua Shan copper mine (pretreated). NF achieved > 90% removal of heavy al., 2007

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metals but low removal efficiency of total conductivity of AMD. RO achieved 14–15% water

recovery efficiency, satisfying the requirements for disposal of heavy metals in wastewater. The

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potential for heavy metal recovery and wastewater reclamation using RO was highlighted.

An RO pilot system (pressure: 65 bar) was used to treat AMD from a coal mine in the Czech Vaclav and

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Republic. It attained total solid retention efficiencies of 88%–98% and showed superior microbial Eva, 2005

removal, meeting the requirements for potable water.

435
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436 6.1.2 Alternative membrane processes

437 6.1.2.1 Membrane distillation

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438 Membrane distillation (MD) is a thermal membrane integrated technology that uses vapor
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439 pressure difference as its driving force (Khayet, 2013, Naidu et al., 2016). In MD, a micro-
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440 porous hydrophobic membrane is applied as a barrier between a hot feed solution (50–70 °C) and

441 cold distillate (20–25 °C). In general, vapor pressure gradient in MD is created by varying the
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442 temperature between the feed and distillate side of the membrane. The hydrophobicity of the

443 membrane enables only water vapor transportation through the membrane pores. The water
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444 vapor is condensed on the cold side. The vapor transfer mechanism in MD allows high rejection
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445 of non-volatile compounds for seawater brine (Choi et al., 2017, Naidu et al., 2015) and

446 wastewater (Naidu et al., 2017a). MD enables the production of high quality fresh water with a

447 water recovery ratio of up to 90% (not limited by pressure operation), promising a near-zero

448 liquid discharge operation for small-scale treatment (Naidu et al., 2014). This is especially

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449 favorable for AMD treatment. Additionally, MD requires minimal electrical energy compared to

450 pressure-operated systems such as RO and NF, while the low thermal requirement can be met by

451 alternative thermal sources such as solar or waste heat (Khayet, 2013).

452

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453 The application of MD for concentrating acid while producing high quality fresh water has been

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454 explored by several previous studies (Tang and Zhou, 2006, Thiruvenkatachari et al., 2006,

455 Tomaszewska et al., 2001, Tomaszewska and Mientka, 2009). These studies established the

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456 suitability of MD for concentrating acid while producing high quality fresh water. Kesieme et al.

457 (2012) tested the performance of MD for treating synthetic AMD using a direct-contact MD

458
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configuration at a feed temperature of 60 °C. The findings indicated that the concentration of
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459 sulfate increased by almost 6 times, from 40 g/L to 245 g/L at stable fluxes in the range of 20–30

kg/m2h-1. More than 99% removal efficiency of sodium and sulfate was achieved with over 80%
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460

461 water recovery. This established the suitability of MD for fresh water production and acid
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462 concentration. It is worth mentioning that both Tomaszewska and Mientka (2009) and Kesieme
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463 et al. (2012) indicated the suitability of MD for concentration of sulfuric acid compared to that of

464 hydrochloric acid. Overall, MD show promising capacity to treat AMD. In fact in a recent study,
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465 Hull et al (2017) adopted an innovative approach of utilizing the thermal condition in MD

466 beneficially as a pretreatment to thermally precipitate Fe from AMD, thereby, minimising

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467 scaling by iron oxyhydroxide. Likewise, Ryu et al (2019) exhibited the flexibility of submerged
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468 MD to be integrated with zeolite to reduce scaling and concentrate valuable metals from AMD.

469 In comparison to conventional MD, submerged MD is beneficial as it minimizes heat losses from

470 recirculation of heated feed solution that occur in conventional cross flow MD mode (Choi et al.,

471 2018). However, to establish the viability of MD for AMD treatment, more long term studies

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472 must be carried out. Factors such as the susceptibility for wetting under acidic condition and

473 gypsum scaling must be evaluated in detail. Further, focus must be placed on pilot scale designs

474 with better energy efficiency such as multi stage MD (Lee et al., 2016), given that low energy

475 efficiency is one of the key reasons that MD has not attained commercialization. Given that

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476 AMD is a sulfur-based acidic solution, this factor is especially important in establishing the

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477 suitability of MD for concentrating AMD, producing fresh water, and potentially recovering

478 metals from the concentrated solution. Upon MD treatment, Kesieme et al. (2012) used solvent

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479 extraction to recover acid and metals from the concentrated solution.

480

481 6.1.2.2 Forward osmosis

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482 Forward osmosis (FO) is an emerging low-energy membrane technology using osmotic pressure,

instead of hydraulic pressure, as the driving force (Cath et al., 2006, Qasim et al., 2015). In FO,
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483

484 hydrostatic osmotic pressure difference is created by placing a highly concentrated draw solution
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485 and a lower concentrated feed solution through a semi-permeable membrane. Fresh water is
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486 extracted from the feed solution to the draw solution. As an alternative treatment process, FO

487 offers substantial advantages of low fouling and low energy requirement compared to pressure-
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488 operated membrane processes such as RO (Cath et al., 2006). This is especially relevant given

489 that pretreatment is essential for RO and NF prior to AMD treatment.

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490
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491 Vital et al. (2018) used FO (Porifera TFC membrane) with NaCl as well as NH4HCO3 as draw

492 solutions for treating AMD obtained from a copper mine in Chile. NH4HCO3 was not favored as

493 a draw solution for AMD treatment as it resulted in high scaling precipitation on the membrane.

494 Using NaCl as a draw solution, FO was able to achieve more than 98% rejection of most ions in

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495 AMD. However, the phenomenon of reverse salt flux was a major drawback of the process,

496 indicating the need for better FO membranes.

497

498 In fact, the limitation of FO in terms of lack of suitable membranes and draw solution dilution

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499 have spurred the development of hybrid FO systems, the combination of FO with conventional

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500 treatment such as bioreactor and NF (Chekli et al., 2016, Thiruvenkatachari et al., 2016). Hybrid

501 systems offer the possibility to increase the efficiency of both FO and conventional treatment

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502 process. The application of a hybrid FO system for AMD treatment could potentially result in

503 enhanced water reuse and resource recovery, as discussed in Section 7.

504
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505 6.1.2.3. Electrodialysis

Electrodialysis (ED) is an efficient electrochemical and membrane based process. It separates

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506

507 ions across cation and anion exchange semi-permeable selective membranes from non-ionic
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508 compounds in an aqueous solution (Luiz et al., 2018, Sadrzadeh and Mohammadi, 2008, Xu and
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509 Huang, 2008). In a typical ED cell, anion and cation exchange membranes are placed

510 alternatively between a cathode and an anode. The cations and anions migrate towards the
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511 respective electrodes on application of a direct current (Sadrzadeh and Mohammadi, 2008).

512 Cations migrate towards cathodes across a cation-exchange membrane. Similarly, anions migrate
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513 toward anodes across an anion-exchange membrane. As a result, the ion concentration in one
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514 compartment increases while that in the other compartment decreases.

515

516 Given that it is a promising process with minimal chemical requirements, the application of ED

517 has been explored for water reuse and recovering resources from seawater (Sadrzadeh and

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518 Mohammadi, 2008), the electroplating industry (Scarazzato et al., 2017), industrial effluents

519 (Luiz et al., 2018) and the acid industry (Cifuentes et al., 2006).

520

521 Buzzi et al. (2013) highlighted the suitability of electrodialysis for AMD treatment, showing that

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522 it can achieve 97% contamination rejection to produce water suited for reuse. Martí-Calatayud et

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523 al. (2014) used ED for treating AMD, with a focus on recovering pure sulfuric acid.

524 Nevertheless, both studies reported the efficiency reduction of ED due to scaling (iron

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525 deposition) on the cation membrane’s surface, indicating compromised membrane life span in

526 long-term applications. This is an important factor given that although ED is a promising

527
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technology, it is not economically competitive as a conventional NF or RO membrane process.
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528 This is attributed to costly membranes such as bipolar type membranes, electrodes as well as the

low life duration of the membranes.

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529

530
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531 6.2 Resource recovery

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532 6.2.1. Recovery of sulfuric acid

533 Acids are widely used in chemical and metal industries for various treatments. In recent times,
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534 the increasing demand for sulfuric acid has been attributed to its application as a leaching agent

535 in copper-cobalt, nickel and uranium industries (Nleya et al., 2016, Simate and Ndlovu, 2014).
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536 Nleya et al. (2016) provided a detailed summary on the industrial applications of sulfuric acid.
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537 The high sulfuric acid contents in AMD renders it to be highly toxic and corrosive. The hazards

538 associated with acidic AMD are highlighted in Section 3. Recovering sulfuric acid from AMD

539 thus offers two advantages: resource recovery and environmental protection.

540

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541 A number of techniques have been utilized to recover various acids from industrial waste

542 solutions, namely electrodialysis (Cifuentes et al., 2006), diffusion dialysis (Wei et al., 2010),

543 rectification (Song et al., 2013), acid retardation (Sheedy and Parujen, 2012), crystallization

544 (Regel-Rosocka, 2010), and solvent extraction (Haghshenas et al., 2009). Amongst these

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545 methods, electrodialysis is especially advantageous as it can achieve highly concentrated and

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546 purified acid (Cifuentes et al., 2006, Simate and Ndlovu, 2014). There are a number of different

547 electrodialysis configurations. Of these, bipolar membrane electrodialysis is especially attractive

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548 for AMD treatment. This is because, compared to conventional electrodialysis, bipolar

549 electrodialysis utilizes the combination of applied electric field with bipolar membrane to

550
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successfully divide cations and anions into separate sections by splitting water into protons and
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551 hydroxides (Davis et al., 2015; Rozoy et al., 2015). In essence, acid in AMD can be separated

from base salts without chemical dosing using bipolar membrane electrodialysis. Martí-
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552

553 Calatayud et al. (2014) established the capacity of electrodialysis to selectively recover sulfuric
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554 acid from AMD due to the technique of ion exclusion. Further, a three-compartment
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555 electrodialysis cell enabled to achieve highly concentrated sulfuric acid from AMD. However,

556 the capacity of electrodialysis decreased owing to scaling/precipitation on the membrane.

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557 Nonetheless, it is worth mentioning that while the recovery of sulfuric acid takes place mainly by

558 transport of sulfate anions through anion-exchange membranes, precipitation of metallic

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559 hydroxides takes place mainly at the surface of cation-exchange membranes. Therefore, simple
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560 solutions could be adopted on the cation-exchange membranes to improve the limitation on the

561 cation portion of the electrodialysis such as surface modification, exchange of cation-exchange

562 membranes by uncharged membranes and pretreatment to remove multivalent cations. Other

563 alternative techniques with promising potential to concentrate and obtain high purity acid are

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564 membrane distillation (Tomaszewska et al., 2001) and freeze crystallization (Etter and Langill,

565 2016, Padhiyar and Thakore, 2013). Nevertheless, the capacity of these technologies for selective

566 recovery of sulfuric acid from AMD is yet to be explored in detail.

567

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568 6.2.2 Recovery of metals

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569 AMD is viewed as an environmental contaminant due to the presence of heavy metals. However,

570 these contaminants also serve as a potential source of valuable metals. Several methods have

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571 been used for the recovery of metals such as Fe, Cu, Zn, and Ni from AMD (Table 2) via

572 chemical, electrochemical, and biological methods (Crane and Sapsford, 2018, Gaikward and

573
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Gupta, 2008, Isosaari and Sillanpää, 2017, Kefeni et al., 2015, Michalkova et al., 2013,
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574 Nordstrom et al., 2017).
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575

576 Chemical methods include oxide and sulfide precipitation, solvent extraction, and metal
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577 reduction such as Cu cementation. Electrochemical processes include

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578 electrowinning/electroplating, electrocoagulation, hydrolysis, electrodialysis, and electrokinetics.

579 Microbiological processes comprise of sulfate reduction as well as reduction of Fe, Cu, and other
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580 metals. Physiochemical processes such as evaporation, reverse osmosis, and ion exchange are

581 also adopted in combination. Coagulation and sedimentation processes are used in certain cases
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582 where unique metal compositions require a specialized treatment system. Aeration and oxidation
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583 are also introduced to improve the efficiency of chemical treatment (Jones et al., 2015).

584 Selective precipitation still remains the main method adopted for the recovery of metals from

585 AMD.

586

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587 Table 2 Selective metal recovery methods from AMD

Recovery methods Description Ref.

Microbial Recovery of Cu followed by that of Ni and Fe was achieved from synthetic Luo et al.,

electrolysis cell AMD with MEC at 1.0 V. High H2 production rate (1.1 m3 m−3 d−1) was 2014

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(MEC) achieved using AMD containing Cu only. The H2 generated allowed offsetting

the energy input of the treatment.

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Biogenic sulfide Cu precipitation as pure CuS (close to 100% efficiency) was achieved using Sahinkaya

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precipitation sulfide transported from anaerobic baffled reactor effluent from synthetic et al., 2009

AMD (containing Cu and Zn only at pH < 2). Zn precipitation (83–98%

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efficiency) was achieved at the second stage.
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Pilot-scale selective A pilot-scale system (100 L tank) achieved 80% pure Cu (as CuS) and Zn (as Oh et al.,
2016
precipitation ZnS) from an AMD solution (90% recovery rate). The recovery rate strongly
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depended on the flow rate and dose of coagulant.

Selective precipitation of metals like Zn, Mg, and Mn using hypochlorite,

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Hypochlorite
followed by RO in a pilot plant treating 950 m3 of AMD and yielding 80%
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addition combined
water recovery at OZ Minerals Century Mine has been reported.
with RO
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Bioreactor (sulfide- Metals were selectively precipitated from an AMD solution using hydrogen Neilly et

reducing bacteria sulfide from sulfate-reducing bacteria in a laboratory pilot-scale system. Cu al., 2013
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with sequential and Zn (as CuS and ZnS) were recovered at pH = 2.8–3.5 while Ni and Fe

precipitation (SSP)) were removed at pH 6.

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Adsorption Metals (Fe, Zn, Mn, and Ca) were recovered from synthetic AMD using Foucher et

adsorption by different types of activated carbons. al., 2001

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Fractional Cu, Fe, Mn, and Zn, were recovered from an AMD solution (80–99% Mohan and

precipitation efficiencies) using a four-step fractional precipitation process. Fe precipitation Chander,

was achieved through H2O2 addition (pH 3.5–3.6) while Na2S addition 2001

enabled the precipiation of Cu and Zn. At pH 8.5, Mn was precipitated.

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Electrowinning and Zn (over 90% purity) was selectively recovered in 2 h using the Chen et al.,

selective sequential electrowinning method with three electrodes (close to 100% efficiency). 2014

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precipitation (SSP) Sulfate-based Cu and Zn (over 95% purity) were recovered by SSP within 12–

24 h (close to 100% efficiency).

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Selective Use of a graphite anode with 120 mA/L achieved highest oxidation rate. Luptakova

precipitation by Cation exchange and anion exchange membranes showed 40-50% Fe losses. et al., 2012

electrochemical

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Cu and Zn were selectively recovered from synthetic AMD by pH adjustments
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reaction using a neutralizing agent through an electric reaction (54.3–70.3% recovery

efficiency).
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Copper Porous copper cathode was used for an electrowinning experiment. Copper Park et al.,

electrowinning powder was produced from the AMD solution. 2015

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Bioreactor (sulfide- Hydrogen sulfide produced in a sulfate-reducing bacteria (SBR) bioreactor Gorgievski

reducing bacteria system enabled the formation of insoluble metal sulfides (Al, Cd, Co, Cu, Fe, et al., 2009

with sequential Mn, Ni, and Zn (75–98% purity)) in the precipitation step (SSP).
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precipitation (SSP))
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588
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589 6.2.3 Rare earth elements

590 In the periodic table, rare earth elements (REEs) include 15 lanthanides sequences starting with

591 lanthanum (La) and including lutetium (Lu), scandium (Sc) (Haque et al., 2014). Often, rare

592 earth yttrium (REY) is also clustered under the series of REEs. These elements are categorized as

593 rare due to their minimal availability in commercially feasible concentrations and because of the
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594 challenges of attaining these elements in pure form through mining separation processes

595 (Kingsnorth, 2011, Skirrow et al., 2013).

596

597 More than 90% of REEs are produced and supplied by China (Kingsnorth, 2011, Skirrow et al.,

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598 2013). As a result of recent restrictive trade action by China, REEs are now considered strategic

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599 minerals, a term that reflects the global susceptibility towards interrupted supplies, and for

600 industries to be supported from consequences of supply interruptions. REEs are in short supply

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601 internationally, with criticality levels ranked at high scores of up to 29 (Skirrow et al., 2013).

602 Both the US and EU have assigned a high rank to REEs in their respective criticality matrixes,

603
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thus expressing the importance in the use and availability or supply risk of these materials (Fig.
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604 5). The demand for REEs is driven by their essential applications in low-energy emission fields

as well as renewable energy and high technology defense-related applications (Table S3).
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605

606
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607 One of the main approaches for managing the demand of REE is to directly recycle spent
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608 materials containing REE such as batteries, permanent magnets and optical glasses (Haque et al.,

609 2014; Binnemans et al., 2013). Meanwhile, secondary sources of extracting REE include
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610 residues from metal and mining production, namely mine tailing, bauxite residue and

611 metallurgical slags. In exploring the potential of extracting REE from water and wastewater
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612 sources, the US department of Energy (Paul and Campbell, 2011) highlighted on the low
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613 concentration of REE (less than 0.01 ppb) in groundwater, lake, river as well as seawater. In

614 comparison to these water and wastewater sources, AMD contain significantly higher

615 concentrations of REE. Details on REE in AMD and its potential extraction viability is discussed

616 in Section 6.2.3.1.

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5.0
Rare
4.5 Earth
4 (high) Rhodium Elements
Manganese
4.0
Indium
Niobium
Impact of supply restrictions

Platinum
Platinum 3.5
Group
Rare-
Elements
3 earth
(PGE)
Copper element 3.0

Supply risk
Nobium

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Tantalum Germanium
Palladium
Magnesium
2.5 Antimony
Gallium Gallium
Vanadium
Titanium
2.0
2 Indium
Lithium Barite Tungsten

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1.5 Flourite
Beryllium (fluorspar)
Graphite
Cobalt Tantalum
1.0
Lithium Rhenium Magnesite Chromium
1 (low) Borate Limestone Vanadium
Tellurium
0.5 Diatomite Perlite Gypsum Bentonite MolybdenumManganese

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Zinc
Clays Silver Iron
Talc Copper Bauxite Nickel
Feldspar Titanium Aluminium
0
1 (low) 2 3 4 (high) 3 4 5 6 7 8 9 10
Economic importance
Supply risk

(a)
U (b)
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617 Fig. 5. Supply demand ranking of REEs in a matrix by (a) US National Academy of Sciences
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618 (NRC, 2008) and (b) European Commission (EC, 2010).

619
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620 6.2.3.1 Distribution of REEs in AMD

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621 Recent discoveries have indicated AMD as a promising source of REEs (Ayora et al., 2016).

Knowledge of REEs in AMD is still very sparse. A few studies have conducted detail sampling
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622

623 and analysis on the behavioral distribution pattern of REEs in AMD (Table 3). Notably, these
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624 studies intended to evaluate the mobility of REEs at mining sites owing to their environmental
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625 toxicity as well as their application as tracers for remediation (Bonnail et al., 2017, Merten et al.,

626 2005). Nevertheless, the findings of these studies established the relatively high accumulation of

627 REEs (generally rich with middle REEs) in AMD compared to natural water bodies, thus

628 providing an important basis for the potential of recovering REEs from AMD.

629
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630 Table 3 Distribution pattern of REEs in AMD

AMD location REEs detected Ref.

Novo Ursk Gold AMD (pH =1.9) contained La (190 µg/L), Ce (470 µg/L), and Nd Myagkaya et

Deposit, Russia (260 µg/L). Higher MREE concentrations compared to those of al., 2016

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LREEs and HREEs were recorded.

Jales, Portugal AMD contained total REEs of up to 70.4 µg/L. Higher MREE Prudêncio et

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concentrations compared to those of LREEs and HREEs were al., 2015

recorded.

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Iberian Pyrite Belt, AMD (pH =2.8 – 3.1) contained 2,846 µg/L of total REEs. Higher Ferreira da

Portugal MREE concentrations compared to those of LREEs and HREEs were Silva et al.,

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noted. 2009
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Iberian Pyrite Belt, AMD contained total REEs of 3,500–7,900 µg/L. Ayora et al.,

Spain 2016
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Mays Swamp, New AMD contained total REEs of up to 3,000 µg/L. Welch et al.,

South Wales, Australia 2009

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Tinto-Odiel Estuary, AMD (pH~2.7) contained total REEs of 621 µg/L (Y, Sc = 31-187 Borrego et al.,

Spain µg/L) 2012

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Jaintia Hills AMD contained total REEs of 714.7 µg/L. Higher MREE Sahoo et al.,

Coalmines, India concentrations (Nd–Gd) compared to those of LREEs were recorded. 2012
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Sitai Coalmine, North AMD (pH=3.61) contained total REEs of 61.21 µg/L (La =7.77 µg/L, Zhao et al.,

China Ce =19.35 µg/L, Nd =12.98 µg/L, Sm = 2.98 µg/L, Gd = 3.78 µg/L, 2007
C

Dy = 4.06 µg/L, and Er = 2.43 µg/L)

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Copper mine, Iran AMD contained total REEs of 30 µg/L to 10,646 µg/L. Higher Sharifi et al.,

MREE concentrations compared to those of LREEs were recorded. 2013

Huelva Estuary, Spain Acidic water (pH =1.66), total REEs > 11,000 µg/L Lecomte et al.,

2017

631

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632 6.2.3.2 Recovery of REEs from AMD

633 AMD contain small quantities of REEs released at low pH conditions (Protano and Riccobono,

634 2002, Ziemkiewicz et al., 2017). A limited number of studies have reported on the possibility of

635 recovering REEs from AMD. It is more likely that they are adsorbed onto metal oxide/hydroxide

PT
636 colloids, forming co-precipitates, or precipitating directly as RE(OH)3, thereby resulting in the

RI
637 scavenging of REEs from AMD (Zhao et al., 2007). Binnemans et al. (2013) carried out a detail

638 review on various approaches to recover REEs from wastewater sources including AMD. The

SC
639 recovery of REEs from aqueous and acidic solutions has been evaluated using ion-exchange and

640 chelating resins such as modified surface mesoporous silica (Yantasee et al., 2009), nanoporous

641
U
silica surface modified with 3,4-hydroxypyridinone (Johnson et al., 2012), chitosan
AN
642 functionalized with EDTA (Roosen and Binnemans, 2014), activated carbon and silica

composites (Ramasamy et al., 2018), porous amine−epoxy monolith (Wilfong et al., 2017),
M

643

644 functionalized magnetic nanoparticles (Polido Legaria et al., 2015), as well as liquid solvent
D

645 extraction (Kumar et al., 2011, Wang et al., 2013, Xie et al., 2014).
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646

647 While extraction by organic solvents is the favored approach for the recovery of REEs, this
EP

648 method is only best applied with concentrated aqueous waste streams, owing to inevitable toxic

649 contamination from the organic solvents (Binnemans et al., 2013). Ayora et al. (2016) analyzed
C

650 the behavior of REEs in AMD using passive remediation treatment (multistage sequential
AC

651 treatment). This treatment method involves mixing AMD with permeable substrates followed by

652 decantation ponds. The study established that no REEs losses occur during schwertmannite (Fe)

653 precipitation; instead, they are retained in basaluminite residues, indicating the economic

654 potential to recover REES from them. However, to the best of our knowledge, only two recent

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655 studies have explored the recovery of REEs from AMD. Pozo et al. (2017) used a novel bio-

656 electrochemical system to treat AMD and demonstrated the capacity of a continuous bio-

657 electrochemical system to precipitate REEs with up to 498 ± 70 mg Y, 166 ± 27 mg Nd, 155 ±

658 14 mg Gd per gram of solid sludge. López et al. (2018), in a recent study, explored the

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659 possibility of concentrating REEs (La, Sm, Pr, Nd, Dy, and Yb) in synthetic AMD using an NF

RI
660 system (polyamide NF270 membrane). The study reported the high rejection of REEs as triple-

661 charged species (M3+) and single-charged species (MSO4+, and M(SO4)2−) based on dielectric

SC
662 exclusion technique of positively charged polymeric NF membrane. All these studies indicated

663 that concentrating and selectively precipitating REEs could offset the cost of novel AMD

664 treatments.
U
AN
665

6.2.4 Viability of metal recovery from AMD

M

666

667 Overall, the viability of metal recovery from AMD must be evaluated on the basis of the metals
D

668 economic value (market price) over the metals importance (such as supply risk and market
TE

669 consumption size) (Fig. 5), the concentration of the metals in AMD; as well as the extraction

670 efficiency. In this regard, compared to the other metals in AMD, REE fall under a high matrix
EP

671 level of sustainable recovery. However, REE exist in significantly lower concentration compared

672 to other major metals in AMD. Therefore, a highly important aspect on the success of REE
C

673 recovery in AMD is an appropriate method for its extraction. It is a challenge to recover valuable
AC

674 REE as: firstly, it is hard to selectively separate them from other dominant metals in AMD; and

675 secondly, they are not easy to precipitate and crystallize using a single method. For instance, the

676 US Department of Energy’s (DOE) National Energy Technology Laboratory (NETL) has set the

677 criteria for an efficient process to achieve at least 2% or 20,000 ppm REE elemental

37
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678 concentrations from a feedstock containing REEs at 300 ppm (0.03%) and such processes must

679 allow environmentally benign recovery. The purity (concentration) of the REE compounds must

680 be at least 90% (DOE, 2018). Integrated processes may provide a better possibility to selectively

681 extract elements with low concentrations as discussed in the subsequent section.

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682

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683 7. Future potential with integrated processes

684 The principal question under consideration is whether alternative AMD treatment methods can

SC
685 compete with their conventional counterparts. Although several alternative treatment approaches

686 have been advocated for AMD treatment and explored in the laboratory, as discussed in Section

687
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6.1.2, none has attained full-scale implementation. Integrating processes by combining
AN
688 conventional and alternative processes may increase the efficiency of the former while

overcoming limitations of the later. Integrated processes have been explored widely for treating
M

689

690 seawater concentrates and wastewater. Some recommended options with potential to treat AMD
D

691 in a holistic and sustainable manner are described in Table 4.

TE

692

693 Table 4 Recommended integrated options for AMD treatment.

EP

Integrated Description Advantages

processes
C

Membrane (i) Potentially favorable for simultaneously

AC

distillation recovering valuable low concentration elements

(MD)-ion (such as REEs) in AMD using selective ion

exchange exchange adsorbent in a single system.

(ii) Increased AMD concentration (while

Simultaneous fresh water production (>98% ion producing high quality water) by MD and thermal

38
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rejection) is possible while concentrating the condition potentially enhances performance of the

solution, with selective recovery of target ion exchange adsorbent.

element (Naidu et al., 2017b). (iii) Reuse capacity of ion exchange adsorbent is

important for reducing operating cost.

PT
MD- (i)MDBR can provide complete retention of non-

RI
bioreactor volatile organics, salts, and microorganisms (high

(MDBR) quality water reuse compared to conventional

SC
MBR) independent of organic residence times and

hydraulic residence times.

U
(ii) MDBR operates at low operating pressures
MDBR process integrates a membrane bioreactor
and moderate temperature, achieving excellent
AN
with MD to simultaneously produce water and
rejection of non-volatile compounds and produces
treat wastewater. Two main operational
high quality permeate that is independent to the
M

configurations are generally adopted: submerged

biological activity. Operation at an elevated
and stepwise (Phattaranawik et al., 2008)
thermophilic biological process allows for greater
D

organic biodegradation, which in turn delays

TE

membrane fouling and wetting, compared to

standalone MD.
C EP
AC

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MD- (i) The combination can achieve selective salt

crystallizer crystallization while concentrating feed solution

(close to zero liquid discharge).

(ii) Scaling on the MD membrane is reduced by

PT
continuous salt crystallization by the integrated

MD-crystallizer process.

RI
(iii) This compact integrated system is suited for

small-scale treatment with low flow rates (such as

SC
AMD), to produce high quality water and recover

valuable metals as salt crystals (requires minimal

U
(Ali et al., 2018; Macedonio et al., 2007)
AN chemicals for salt precipitation)

Forward (i) FO can reduce NF fouling issues associated

osmosis- with AMD treatment (as discussed in Section

nano 6.1.1).
M

filtration (ii) AMD (low osmotic pressure) is highly

(FO-NF) suitable as a feed solution for FO.

D

(iii) NF can increase standalone FO performance

TE

Feed and draw solution flow tangentially to FO by continuously maintaining draw solution
membrane. Water molecules transport from feed concentration and reducing reverse salt flux
EP

solution (low osmotic pressure) to draw solution (iv) NF permeate is suitable for water reuse
(high osmotic pressure) due to osmotic pressure purposes.
C

difference. NF produces permeate (suited for

AC

reuse) from diluted draw solution (Chekli et al.,

2016, Zhao et al., 2012).

694

695 8. Conclusions

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696 The formation of AMD, a metal-rich acid solution, poses major environmental and economic

697 challenges for the mining industry. The selection of a suitable AMD remediation method (or a

698 few methods combined together) unvaryingly relies on geographical site-specific settings, such

699 as resource availability, constituents in the water, treatment targets, associated risk, and the

PT
700 desired end use of the affected site. The varying effectiveness of current AMD remediation

RI
701 treatments applied at mining sites is specifically attributed to aspects such as regular acidity load

702 of AMD, concentration of metals and flow rate. Operation knowledge and experiences from

SC
703 successful remediation cases at actual mining sites and an understanding of challenges faced will

704 help in the effective management of AMD. It is increasingly challenging to dispose sludge

705
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containing heavy metals produced from AMD management. These factors have led to much
AN
706 emphasis on exploring more sustainable treatment options for reuse and recovery, given that

AMD is now considered a new source for the recovery of REEs. Membrane and alternative
M

707

708 treatment options can produce high quality water for reuse. Nevertheless, high cost, brine
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709 management, membrane fouling (necessitating pretreatment), and membrane lifespan remain
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710 challenges for achieving effective full-scale AMD treatment. Integrated processes offer the

711 possibility to achieve sustainable AMD treatment by increasing the efficiency of conventional
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712 processes while overcoming the limitations of alternative ones.

713
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714 Acknowledgements
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715 The authors acknowledge the support received for this study from Centre for Technology in

716 Water and Wastewater, UTS Early Career Researcher Fund.

717

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Highlights

• Acid mine drainage (AMD) is a global environmental and economic challenge.

• Current AMD remediation applied at real sites and its limitations are highlighted.

• AMD challenges must be addressed through sustainable treatment approaches.

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• Water reuse and valuable resource recovery potentially offset AMD treatment cost.

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• Integrated processes using membranes are prospective approaches for AMD treatment.

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