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Science of the Total Environment 659 (2019) 1415–1427

Contents lists available at ScienceDirect

Science of the Total Environment

journal homepage: www.elsevier.com/locate/scitotenv

Review

Evaluation survey of microbial disinfection methods in UV-LED water


treatment systems
Xiaoling Li a, Miao Cai a,⁎, Lei Wang a, Fanfan Niu a, Daoguo Yang a,⁎, Guoqi Zhang a,b
a
School of Mechanism and Electrical Engineering, Guilin University of Electronic Technology, Guilin 541004, China
b
Delft Institute of Microsystems and Nanoelectronics (Dimes), Delft University of Technology, Mekelweg 6, 2628CD Delft, the Netherlands

H I G H L I G H T S G R A P H I C A L A B S T R A C T

• The latest researches on ultraviolet


light-emitting diodes (UV-LEDs) for
water disinfection are reviewed.
• The disinfection mechanism by UV-
LEDs is discussed in detail.
• The influence rule of UV-LED light
source system parameters is illustrated.
• The influence rule of UV-LED water
treatment system settings is also pre-
sented.
• Conclusions and future suggestions for
UV-LEDs water disinfection are
proposed.

a r t i c l e i n f o a b s t r a c t

Article history: Ultraviolet (UV) disinfection is an early discovered technology that is currently and widely used for water treat-
Received 14 August 2018 ment and food hygiene treatment. A newly emerging technology of UV disinfection, that is, UV light-emitting di-
Received in revised form 22 December 2018 odes (UV-LEDs), has aroused considerable research attention. UV-LEDs feature numerous advantages compared
Accepted 22 December 2018
with traditional UV mercury vapor lamps and are expected to replace traditional UV lamps. Researchers currently
Available online 24 December 2018
perform studies to obtain data and develop methods for UV-LED water treatment systems. This article analyzes
Editor: Paola Verlicchi the latest research status and discusses the types of inactivation factors, such as the wavelength selectivity of UV
light source, control of UV dose, effect of inactivation rate constant (K) (cm2/mJ), working mode of water sample,
Keywords: external auxiliary system, and UV sensitivity of pathogenic bacteria in water. The wavelengths of approximately
Ultraviolet disinfection 260 and 280 nm normally feature strong inactivation characteristics. When compared with the approximately
Ultraviolet light emitting diodes (UV-LEDs) 260 nm wavelength chip, the around 280 nm wavelength chip proves to be a better choice as its higher wave-
Water treatment length light power can result in faster disinfection capacity of bacteria. UV dose can also be used as the reference
Inactivated effects value for disinfection of drinking water, whereas the inactivation rate constant (K) (cm2/mJ) varies with different
Standardization
microorganism internal structures. Changing the working mode or adding an auxiliary system can also enhance
the inactivation effect in water treatment system settings. In addition, we can compare the inactivation capacities
of several pathogens as follows: ΦX174 N Escherichia coli N T type bacteriophage N Bacillus subtilis N MS2 or Qβ
N human adenovirus. The in-depth investigation and discussion of inactivation factors and the mechanism of ac-
tion in UV-LEDs water treatment systems will establish a more efficient UV-LED disinfection method in the

⁎ Corresponding authors.
E-mail addresses: caimiao105@163.com (M. Cai), daoguo_yang@163.com (D. Yang).

https://doi.org/10.1016/j.scitotenv.2018.12.344
0048-9697/© 2018 Elsevier B.V. All rights reserved.
1416 X. Li et al. / Science of the Total Environment 659 (2019) 1415–1427

future, provide a guiding direction, and promote the standardization and normalization of pathogen inactivation
mechanism in UV-LED water treatment systems.
© 2018 Elsevier B.V. All rights reserved.

Contents

1. Background. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1416
2. UV disinfection mechanism . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1417
3. Influence rule of disinfection methods. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1419
3.1. Influence of UV-LED light source system parameters on inactivation mechanism . . . . . . . . . . . . . . . . . . . . . . . . . . . 1419
3.1.1. Wavelength of UV-LEDs. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1419
3.1.2. UV dose . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1420
3.1.3. Inactivation rate constant (K) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1422
3.2. Influence of UV-LED light source on water treatment system settings . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1423
3.2.1. Working mode of water sample . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1423
3.2.2. Water treatment reactors . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1424
3.2.3. Auxiliary system . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1425
4. Conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1425
Acknowledgments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1426
References. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1426

method for water disinfection (Bowker et al., 2011; Kheyrandish et al.,


Nomenclature 2017a; Kim et al., 2017). UV irradiation has drawn considerable atten-
tion in water disinfection and food industries, especially in water treat-
CPD Cyclobutane pyrimidine dimer ment applications (Kim et al., 2017). UV disinfection has also been
A Adenine recommended as a substitute for chemical additives for surface water
G Guanine treatment according to a US Environmental Protection Agency report;
T Thymine it can effectively inactivate viruses at 4 log reduction in surface water
C Cytosine in water disinfection systems (USEPA, 2006). To date, more than 7000
MP Medium-pressure mercury lamp municipal UV disinfection installations exist worldwide (Muller,
LP 254 nm Low-pressure mercury lamp 2011), and small household UV disinfection systems are also available
E. coli Escherichia coli (Brownell et al., 2008). UV disinfection equipment from the global mar-
B. subtilis Bacillus subtilis ket is expected to reach $2.8 billion by 2020 (Allied Analytics LLP, 2014).
B. pumilus Bacillus pumilus Conventionally, UV light is generated from mercury lamps, including
L. pneumophila Legionella pneumophila low-pressure (LP) mercury lamps, which emit nearly monochromatic
P. aeruginosa Pseudomonas aeruginosa UV light at a wavelength of 254 nm, and medium-pressure lamps
HAdV Human adenovirus (MP), which emit a polychromatic spectrum with various wavelengths
K Inactivation rate constant (Bolton and Cotton, 2008). However, UV mercury lamps are packaged
DOM Dissolved organic matter by glass, which is fragile. UV mercury lamps easily cause mercury spills
in the external environment, releasing harmful vapors into the air for
weeks or years. In recent years, a new friendly method was developed
to generate UV light, that is, UV light-emitting diodes (UV-LEDs).
Vilhunen et al. (2009) used UV-LEDs at 269 and 276 nm wavelengths
as an optimal method for bacterial disinfection; other studies also sup-
1. Background port that UV-LEDs can work effectively in disinfection. However, UV-
LEDs feature drawbacks: the UV-LED chip is prone to lattice defects, dif-
The safety of drinking water remains an important issue worldwide, ficult to develop, and features low internal light efficiency (Wang et al.,
especially in most developing countries and numerous rural areas (Song 2015; Yan et al., 2017). The chip packaging is also prone to various prob-
et al., 2016). Drinking water is easily polluted by major pollutant lems, such as UV aging, internal interconnection failure, interface shed-
sources such as biological pollutants, which include various pathogenic ding, wire bonding failure, and light decay failure (Kheyrandish et al.,
microorganisms, easily causing the spread and epidemic of water-borne 2017a, 2017b; Beck et al., 2017; Luo et al., 2016; Arik et al., 2004; Lu
diseases (Wang et al., 2009). Polluted drinking water will result in et al., 2016; Yang et al., 2016a, 2016b), and notable challenges occur in
proliferation of various human enteric viruses, including hepatitis A the application mechanism research and development (R&D) design
virus, rotavirus, and norovirus. Human enteric viruses may cause severe of encapsulated UV-LED products; these challenges include improving
diseases, such as hepatitis, poliomyelitis, and meningitis (Kim et al., the performance of UVC-LED reactors, creating a predictive model that
2017). can predict the average fluence rate, and developing measurement
In 2000, the US Food and Drug Administration approved ultraviolet techniques and accurate protocols for measuring and controlling the
(UV) disinfection as an effective method that can inactivate the replica- UV-LED output. Still, UV-LED chip R&D technology achieves continuous
tion of pathogens and spoilage microorganisms in food, water, and progress, although the epitaxial slice with a short wavelength is difficult
beverages. UV disinfection is a chemical-free process, generates no by- to develop, and lattice failures within the chip are less manageable.
products, and hardly affects the nutritional values of food. Disinfection Short wavelength development has also shown remarkable progress.
by UV radiation features no risk of overdosing, making it a viable Chips with wavelengths of below 280 nm have been developed, with
X. Li et al. / Science of the Total Environment 659 (2019) 1415–1427 1417

200 nm to 280 nm being the most useful disinfection bands. In addition, 2. UV disinfection mechanism
chip packaging module output efficiency is constantly improved in chip
encapsulation mode, including single chips. The multiple-chip array People historically discovered DNA or RNA as the key target in vari-
module is also commonly used today; it remarkably improves the out- ous organisms; UV disinfection causes the death of organisms when
put power of the entire device. Disinfection application products made their DNA or RNA absorbs UV light (Hijnen et al., 2006). Numerous stud-
by UV-LED packaging constantly emerge in the market. UV-LEDs feature ies were conducted on mutagenic DNA lesions induced by UV irradia-
more advantages compared with UV mercury lamps in a number of tion. According to microbiological experiments, mutagenic DNA
ways; UV-LEDs possess an adjustable wavelength and can emit lesions induced from UV irradiation belong to two major classes,
radiation from 210 nm up to visible light and are promising UV radiation namely, cyclobutane pyrimidine dimers (CPDs) and 6–4 photoproducts;
sources (Shur and Gaska, 2010). UV-LEDs cause no disposal problem although the possibly existing Dewar valence isomers are extremely
(mercury-free), leave a small footprint (flexible architecture), are low to count, CPDs are the most abundant and compose around 75%
mechanically robust, and possess an instant on–off functionality of UV-induced DNA damage products in mutagenic DNA lesion inducers
(high-frequency response), low voltage, low power requirements, and (Sinha and Häder, 2002). Fig. 1 shows the construction and generative
long lifetimes (reduced frequency of replacement) (Würtele et al., process of cyclobutane thymine pyrimidine dimers (Bolton and
2011). Cotton, 2008).
UV-LEDs feature numerous advantages, but owing to the current Maximum UV light absorption from DNA is reached at a wavelength
overall technical difficulties, various aspects remain underdeveloped. of ~260 nm; however, in most cases, the absorption peak wavelength
Most UV-LED applications are still in the state of R&D, and no standard distribution, which varies among organisms, becomes dependent on
measurement scheme and description determine how UV-LEDs can the target organism (Bolton and Cotton, 2008; Chen et al., 2009). For ex-
achieve the disinfection mechanism. Meanwhile, the measurement ample, Chen (2009) presented that Bacillus subtilis spores feature two
technology of traditional mercury lamp has developed. As early as absorption maxima: one below 240 nm and another around 270 nm.
2003, Bolton and Linden have developed a standardized protocol and Cabaj et al. (2002) and Mamane and Linden (2005) obtained similar re-
obtained accurate and consistent results for microbiological and photo- sults and showed that the wavelength of fluence inactivation response
chemical experiments by determining an accurate UV fluence (Bolton curves totals 254 and 279 nm, respectively. Different target organisms
and Linden, 2003). A protocol was also developed for measuring UV exhibit different sensitivities under UV irradiation (Aoyagi et al.,
mercury lamp output through researching different parameters 2011). Although the genetic material of pathogens is either DNA or
(Sasges and Robinson, 2005). Later, more practical protocols were intro- RNA, they also contain other components, such as proteins and a cell
duced, and different industry participants, including the International membrane. Thus, we should perform various analyses for complex
Ultraviolet Association, showed much interest (Lawal et al., 2008; organisms.
Adam et al., 2010). However, these measurement protocols were devel- The action spectrum arises primarily from the DNA that absorbs UV
oped for UV mercury lamps and were unsuitable for UV-LEDs, which photon and matches the relative absorbance of DNA extracted from an
possess different structures and output specifications (Kheyrandish organism; for instance, the action spectrum of S. typhinium matches
et al., 2017a). Therefore, a measurement and analytic system for UV- well with the relative absorbance of the DNA extracted from the organ-
LED must be launched. A number of scholars carried out studies on var- ism (Chen et al., 2009). The absorbance of other components to photons,
ious aspects of UV-LED water treatment in recent years. Consequently, a rather than the DNA in spores, are also non-negligible, as these compo-
standard protocol should be established to accurately control and mon- nents maybe involved in the inactivation effect by germicidal UV light
itor the output of UV-LEDs and assess the consistency of UV-LEDs with (Chen et al., 2009).
an accurate and reliable method in different experiments and devices; The formula of the first-order model of Chick–Watson (Hijnen et al.,
protocols must also be developed for measuring and controlling UV- 2006) is described by Eq. (1):
LED output, radiation profile, radiant power, and UV dose for water dis-
infection applications (Kheyrandish et al., 2017a, 2017b; Simons et al., LogðN0=NÞ ¼ K UVdose ð1Þ
2014). Other researchers investigated the synergistic effects of dual
wavelength to compare log inactivation values (Beck et al., 2017; where N0 and N refer to the number of colonies (CFU/mL) before and
Chevremont et al., 2012b). Scholars also showed interest in adding aux- after UV irradiation, respectively; UV dose (mJ/cm2) is the fluence at a
iliary equipment, such as an ultrasonic pretreatment system, for achiev- given wavelength; K (cm2/mJ) is the proportional coefficient used to de-
ing better antibacterial rate (Zhou et al., 2017; Andrej et al., 2014). scribe inactivation, that is, the inactivation rate constant (Li et al., 2017).
Studies on disinfection of air surfaces, such as by an automatic disinfec- The time-based and fluence-based inactivation rate constants (K) by
tion stethoscope device made by UV-LED lamp, solved the problem on UV-LED for Escherichia coli are higher than those for other species, and
transmission of hospital pathogens through the stethoscope (Messina their differences among viruses show statistical significance (Oguma
et al., 2015; Messina et al., 2016; Messina et al., 2018). The UV-LED sys- et al., 2016). Considering the order of sensitivity among four microbial
tem will improve gradually, but forming a comprehensive, standard- species, namely, E. coli K12 IFO 3301, Qβ, MS2, and human adenoviruses
ized, and normalized UV-LED disinfection mechanism remains (HAdV), E. coli is the most sensitive, whereas HAdV are the most resis-
extremely urgent. tant, similar to the order of sensitivities observed for an LP UV lamp in
This article thoroughly analyzes the latest research status, with dis- the work of Hijnen (Hijnen et al., 2006; Rattanakul et al., 2014;
cussion by horizontal and vertical comparisons, and determines the in- Oguma et al., 2016). However, UV sensitivity is distinguished in terms
terconnections among inactivation factors and the mechanism of action of the generic material, which can be single- (ssDNA) or double-
from the influence rule of UV-LED water treatment systems. We will stranded DNA and single- (ssRNA) or double-stranded RNA, which is
conduct in-depth investigation and discussion to highlight the disinfec- inherited by viruses, such as the ssDNA of ΦX 174 viruses or ssRNA of
tion mechanism to gain insights into the related inactivation mecha- MS2 and Qβ viruses. The UV sensitivity of viruses has also been evalu-
nism. As a result, researchers can expand the relevant design and ated by the inactivation rate constant (K) (cm2/mJ) (Hijnen et al.,
research work in UV-LED water treatment systems. This paper also ex- 2006; Song et al., 2016). MS2 and Qβ yield similar inactivation rate con-
plores the methods of deep UV-LED disinfection for the establishment stants (K) (cm2/mJ) values and show no significant difference regard-
of a more efficient UV-LED disinfection technique in the future, provides less of the kind of treatment condition. However, ΦX 174 exhibits
a guiding direction, and promotes the standardization and normaliza- statistically high UV sensitivity and inactivation rate constant (Kim
tion of pathogen inactivation mechanism in UV-LED water treatment et al., 2017). Regarding the exploration of different species in terms of
systems. inactivation capacities or anti-UV ability, biological inactivation
1418 X. Li et al. / Science of the Total Environment 659 (2019) 1415–1427

Fig. 1. Double-stranded DNA chain showing how the formation of thymine dimers disrupts the structure chain (top); photochemical dimerization of two thymine bases (bottom) (Bolton
and Cotton, 2008).

capacities, which mean the capacities of microorganism to be formation of genomic damages, which are reparable by DNA repair
inactivated by UV light, must be compared. The exploration of each spe- mechanisms; on the other hand, UVA inactivates microorganisms, caus-
cies in terms of the absorption wavelength will determine the optimum ing diverse irreparable damages in cells by promoting the formation of
disinfection wavelength for each microorganism. active species (Friedberg et al., 1995; Oguma et al., 2013). UVA radiation
UV-LEDs comprise UVC (200–280 nm), UVB (280–315 nm), and can destroy the cell membrane and other cellular components by pro-
UVA (315–400 nm). The inactivation mechanism of UVC irradiation is ducing hydroxyl and oxygen radicals to damage proteins (Chevremont
based on the absorption of UV photons from the genetic material and et al., 2012a). DNA damage can be repaired by the enzyme photolyase
produces dimers that can inhibit the transcription and replication of with UVA radiation, but no reported evidence discusses the damage of
genes from cells (Bolton and Linden, 2003; Oguma et al., 2002). How- bacterial membranes that can be repaired by UVA radiation.
ever, most DNA repairs, including photoreactivation and dark repair, Chevremont et al. (2012a) showed that coupling UVA and UVC can be
occur under low UV doses. In photoreactivation repair, which is the more effective by using the germicidal effect of UVC and greater pene-
major process of DNA repair, photoenzymes are specifically identified trating capability of UVA; this coupling increases the efficiency of micro-
as enzymes that can repair CPD dimers by absorbing light energy in bial inactivation owing to the lack of possibility to repair the damage
the 310–480 nm wavelength (UVA or partial visible light); the dark re- when bacterial membranes can be destroyed after UVA exposure
pair, which requires no light, replaces damaged DNA nucleotides with (Chevremont et al., 2012a). UV-LEDs with wavelengths at the coupling
undamaged DNA and causes minimal effects (Bolton and Cotton, range of UVA and UVC exhibit higher polyphenol oxidase inactivation
2008). Although UVA may undergo photoreactivation, recent results efficiency than traditional LP mercury lamps. Compared with UVC irra-
showed that UVA radiation mechanism can cause inactivation of micro- diation and thermal treatment, UVC irradiation from the coupling wave-
organisms when coupling UVA and UVC (Chevremont et al., 2012a). length by UVA and UVC achieved better color preservation of cloudy
Bactericidal effects from UVC and UVB may be similarly based on the apple juice (Akgün and Ünlütürk, 2017). Furthermore, the light from
X. Li et al. / Science of the Total Environment 659 (2019) 1415–1427 1419

UVA radiation, although not absorbed by DNA, can produce hydroxyl disinfection systems: wavelength, UV dose, and inactivation rate
radicals to damage protein bacterial membranes and inactivate micro- constant (K) (cm2/mJ).
organisms (Chatterley, 2003; Chevremont et al., 2012b). UV dose is
the most crucial factor regardless of whether using UVC, UVB, or UVA, 3.1.1. Wavelength of UV-LEDs
whose effects remarkably differ at low UV doses. B. subtilis and Salmo- Wavelength is a key factor in microbial disinfection mechanism of
nella typhi undergo “shoulder” self-repair at low UVC doses (Chen UV systems. From the UV source disinfection, the wavelength of
et al., 2009). Low UVA radiation easily causes photoreactivation. 253.7 nm can be assumed as the most effective when using traditional
Thus, we should develop a multivariate approach to specify the most mercury lamps for disinfection (Bolton and Cotton, 2011). However,
influential factors of inactivation. Several factors affect inactivation mercury lamps perform disinfection using two ways: LP and MP. MP
yields; such factors include bacterial density, pH, UV exposure time, is mixed with multiple emission peak wavelength. Determining the
and the single wavelength or coupling wavelength of chips most effective wavelength from MP presents difficulty. Emission peaks
(Chevremont et al., 2012b). We will thoroughly analyze and discuss from LP concentrate at around 254 nm wavelength, whereas the opti-
their mechanism of action. mal germicidal wavelength serves as the center wavelength at
253.7 nm (Bolton and Cotton, 2011). As UV-LEDs can emit light of ad-
justable wavelength and provide insights into the effect of wavelength
3. Influence rule of disinfection methods
on disinfection, the development of UV-LED will enable the more qual-
itative analysis of microbial inactivation.
This article divides UV-LED sterilizing water treatment systems into
Regarding DNA absorbance relation curves, the wavelength at
two parts: the UV-LED light source system, which is a key part and the
260 nm exhibits the largest absorbance (Bolton and Cotton, 2008).
most influential factor affecting the efficiency of the whole system;
However, in the actual experiment on microorganism inactivation by
water treatment system, which receives the UV-LED light source and
UV-LEDs, different microbes showed different absorption curves, with
serves as the reaction location where microbes are killed off and
each microorganism presenting inconsistent disinfection abilities. The
whose setting shows a relationship to disinfection results.
absorbance values at 260 and 280 nm indicate strong inactivation char-
acteristics. When the inactivation capacities of different microorgan-
3.1. Influence of UV-LED light source system parameters on inactivation isms were compared in terms of UV dose response, the dose response
mechanism per log inactivation of each species at the wavelength of ~260 nm was
consistently less than that at 280 nm. For example, Bowker et al.
UV emission light source system is the main factor affecting disinfec- (2011) observed that the dose responses per log inactivation for MS2
tion. According to the inactivation mechanism, disinfection of microor- reached 26.07 and 28.57 mJ/cm2 at wavelengths of 255 and 275 nm, re-
ganisms in UV water treatment system prevents the replication and spectively. Oguma and Surapong (2018) declared that a 265 nm wave-
transcription of microbial genetic materials by absorbing UV photons length yielded a lower dose response in per log inactivation of E. coli, B.
and generating polymers. In UV water disinfection systems, the most subtilis spores, Legionella pneumophila, Pseudomonas aeruginosa, and Qβ
common light source transmitter systems include traditional mercury than the 280 nm wavelength. Similarly, Beck et al. (2017) discovered
lamps and emerging UV-LEDs. However, the large and bulky UV mer- that a 260 nm wavelength resulted in a lower dose response per log in-
cury lamp installation may be replaced by compactly structured UV- activation for B. subtilis, B. pumilus, and HAdV2 than the 280 nm wave-
LEDs, which are very marketable and show promise owing to their length. Among the tested wavelengths, the UV-LED wavelength of
small and flexible appearance. The UV-LED chip encapsulation features ~260 nm achieved the highest bacterial inactivation regardless of the
multiple packaging forms: single chip and multiple-chip array. Fig. 2 bacterial species, as proven by the highest UV absorbance of nucleic
shows the UV-LED light source system comprising a basic circuit, acids at ~260 nm (Harm, 1980; Bolton and Cotton, 2008; Oguma and
power supply, and four UV-LED chips packaged in the 1, 2, 3, and 4 po- Surapong, 2018). However, we still cannot affirm that the 260 nm UV-
sitions, respectively. The wavelength of UV-LED chips can be selected as LEDs result in more desirable disinfection benefits.
needed. We can select chips with the same or different wavelengths for At the current level of technology, the 280 nm wavelength is an op-
setting the UV-LED chip number or wavelength depending on the situ- timum choice to achieve high inactivation efficiency with minimum en-
ation analysis. ergy consumption. Oguma observed that the 280 nm UV-LEDs can
In this part, we can analyze and subsequently determine the optimal achieve a high inactivation rate constant and feature the lowest energy
light source, optimal efficiency, and disinfection effect of UV-LED water consumption to achieve 3 log inactivation in the microbial species
treatment disinfection systems. This section focuses on three aspects tested at 265, 280, and 300 nm (Oguma and Surapong, 2018). By com-
to further explore the mechanism of UV-LED water treatment paring disinfection efficiencies, another group also noted that the

Fig. 2. Experimental UV-LED light source system.


1420 X. Li et al. / Science of the Total Environment 659 (2019) 1415–1427

280 nm wavelength is more suitable than 255 nm for water purification Bunsen–Roscoe reciprocity law, which states that the photochemical ef-
systems because the power produced from the external quantum effi- fect depends only on the total energy dose, that is, the origin of exposure
ciency at 280 nm reached more than 10 times that obtained at time and fluence rate (Murata and Osakabe, 2013). Sommer et al.
255 nm (Aoyagi et al., 2011). Würtele reported the higher light power (1998) have verified the existence of same log inactivation under the
output and inactivation capacities at 282 nm than those at 269 nm. Al- same product of fluence rate and exposure time when they have
though the 269 nm UV-LEDs exhibited a better germicidal effectiveness, inactivated the bacteriophages MS2, ΦX174, and B40-8 by mercury
the 282 nm UV-LEDs caused a significantly better spore inactivation for UV lamps. They also observed that E. coli inactivation deviated from
the same time span and input power owing to the higher photon output the reciprocity law and showed a higher log inactivation in a higher
(at the same current) of the 282 nm UV-LEDs (Würtele et al., 2011). In fluence rate and shorter exposure time than under a lower fluence
the range of the UV disinfection band, a higher wavelength light power rate and prolonged exposure time despite using the same total UV
can result in faster disinfection capacity of bacteria; lower wavelength fluence (UV dose). This phenomenon could indicate that UV disinfection
peak values are close to DNA absorbance relation curves, but lower- depends on both photochemical reactions and biological processes
wavelength UV-LEDs are more effective when considering light power (Harm, 1980). Then, as the deviation from the Bunsen–Roscoe reciproc-
(Vilhunen et al., 2009). The selection of UV-LED wavelength shows po- ity law may occur on certain microorganisms, such as E. coli, the biolog-
tential for future applications in water disinfection systems equipped ical processes induced by UV radiation may vary with different
with UV-LEDs (Oguma and Surapong, 2018). Coupling wavelength has microorganisms; thus, certain organisms may be more sensitive to the
also been widely used in discussion in recent years; however, the ob- fluence rate compared with the others (Song et al., 2016). Meanwhile,
tained results vary, and the total power of coupling wavelength is infe- a closer radiation distance causes larger radiation flux. However, the
rior compared with the use of single-type UV-LEDs for disinfection; current investigations about radiation distance from UV emission
although further investigation is needed, other applications by wave- sources to water surface are lacking. We probably cannot perform an
length combination yield better disinfection effect and optimize the ad- in-depth research owing to the current technical level, which is still at
vantages of different types of wavelength (Akgün and Ünlütürk, 2017). the stage of close-range surface irradiation or near-surface water sam-
ple radiation of water-body experimental research. However, with in-
3.1.2. UV dose creasing UV-LED external quantum power, radiation distance will
UV dose is another key factor in UV-LED water disinfection systems. soon become a focus of research, especially in the design of various
UV dose is not only directly produced by UV-LEDs but can also be af- products. The depth of water sample is discussed in several articles
fected by the settings of parameters and related instruments. UV dose and is also the most important factor for UV transmittance. Therefore,
is equal to the product of UV radiant flux, exposure time, attenuation setting of different parameters of water sample depth may yield differ-
factor, and radiating surface; the corresponding formula can be ent results in various systems.
expressed as follows: UV dose = UV radiant flux ∗ exposure time ∗ at- First, when comparing the UV doses per log inactivation of different
tenuation factor / (radiating surface). In the formula, UV radiant flux, microorganisms, the same wavelength must be ensured. Table 1 shows
which is also known as radiant power, is defined as the radiant energy the detailed analysis of each wave band, which can be used as a refer-
passing through a section in unit time when light radiates outward ence frame that estimates the UV dose for a specific logarithmic inacti-
and is expressed in watts (W); UV dose is defined as the radiant energy vation number. We can compare the inactivation capacities of different
received per unit area of receiving ionizing radiation (mJ/cm2) and rep- microorganisms from the UV dose response. At a wavelength of 255 nm,
resents the absorbed dose of the water sample from the UV transmitter bacteriophages MS2 and Qβ present similar UV doses of 12.81 and
to the water treatment reactor. This system involves complex attenua- 12.5 mJ/cm2 for per log inactivation respectively, indicating the require-
tion factors, including water, reflection, divergence, and sensor factors ment for more UV dose to be inactivated compared with E. coli
(Bolton and Linden, 2003). Therefore, UV dose is not a real value but (3.33 mJ/cm2), T7 (5.13 mJ/cm2), and ΦX174 (1.73 mJ/cm2). The inacti-
an approximation. vation capacities of E. coli are higher than that of T7 but lower than that
If we only control the UV radiation flux, the experimental results will of ΦX174 (Bowker et al., 2011; Aoyagi et al., 2011). Similar results were
significantly vary owing to the different radiation times, radiation dis- achieved by Aoyagi et al. (2011), who showed the strong and weak re-
tances, and intensities. LP features a high radiation flux rate when sistances of MS2 and ΦX174, respectively, and almost the same inacti-
only the control dose is kept constant, but radiation time, radiation dis- vation capacities of MS2 and Qβ. At a wavelength of 260 nm, the dose
tance, and radiation intensity differ between LP and UV-LEDs (Würtele responses per log inactivation of MS2 and HAdV2 reach 15.15 and
et al., 2011). LP emits a parallel light, whereas the UV-LED lamp is a 30.5 mJ/cm2 respectively; thus, the inactivation capacities of MS2 are
point light source that emits a diffused light depending on the viewing higher than that of HAdV2, as observed by integrated cell culture quan-
angle. Different from LP, radiation intensity is defined as the radiant titative polymerase chain reaction, but lower than that of E. coli K12
flux leaving the point source within a given direction cube in the UV- (ATCC 29425), which requires 1.5 mJ/cm2 dose responses per log inac-
LED light source system. Considering the most influential factors, we tivation (Beck et al., 2017). At a wavelength of 265 nm, the dose re-
control the equal UV radiation dose, where under a specific circum- sponses per log inactivation of Qβ, B. subtilis, and E. coli IFO 3301 total
stance, the same attenuation factor is considered. Exposure time is 39, 28, and 6 mJ/cm2 respectively; thus, the inactivation capacities of
closely associated with flux and dose, that is, a larger radiation flux B. subtilis are higher than that of Qβ but lower than that of E. coli IFO
will result in short exposure time. Furthermore, several researchers ob- 3301 (Oguma and Surapong, 2018). At a wavelength of 266 nm, bacte-
served that high radiation flux and short exposure time may result in a riophages MS2 and Qβ show specific UV doses for per log inactivation at
higher logarithmic inactivation compared with low flux and long expo- 1.29 mJ/cm2, and their doses are higher than that of ΦX174, which re-
sure time as prolonged exposure time may cause microbial aggregation, quires a dose response per log inactivation of 0.14 mJ/cm2 (Kim et al.,
which leads to decreased inactivation (Song et al., 2016; Zhou et al., 2017). At a wavelength of 275 nm, UV doses for per log inactivation
2017). The higher effectiveness of 275 nm is also proposed to be more from MS2, T7, and E. coli reach 28.57, 4.26, and 2.37 mJ/cm2, respec-
effective for E. coli inactivation in a higher fluence rate and shorter expo- tively; thus, the inactivation capacities of T7 are below that of MS2
sure time to reach the same UV dose than the combination of a lower and lower than that of E. coli (Bowker et al., 2011). Furthermore, at
fluence rate and longer exposure time owing to the higher output 280 nm, the inactivation capacities can be compared as follows:
power from the 275 nm UV-LEDs (Bowker et al., 2011; Harm, 1980; ΦX174 N E. coli N B. subtilis N MS2 or Qβ N HAdV2 (Aoyagi et al., 2011;
Sommer et al., 1998). Thus, when we control the same UV radiation Oguma et al., 2013; Beck et al., 2017; Oguma and Surapong, 2018). In
dose, a larger radiation flux may result in better disinfection effect. Var- LP environment, the inactivation capacities are ordered as follows: E.
ious studies have also hypothesized that UV inactivation follows the coli K12 IFO 3301 N T1 N B. subtilis N MS2 N HAdV2 (Rodriguez et al.,
X. Li et al. / Science of the Total Environment 659 (2019) 1415–1427 1421

Table 1
UV dose responses for per log inactivation.

Wavelength (nm) Microorganism Log inactivation UV dose (mJ/cm2) Dose responses per log inactivation (mJ/cm2) Reference

255 E. coli 2.7 9 3.33 Bowker et al., 2011


255 MS2 3.2 41 12.81 Aoyagi et al., 2011
255 MS2 2.3 41 26.07 Bowker et al., 2011
255 Qβ 2.4 30 12.50 Aoyagi et al., 2011
255 T7 3.9 20 5.13 Bowker et al., 2011
255 ΦX174 3.7 6.4 1.73 Aoyagi et al., 2011
260 E. coli K12(ATCC 29425) 3 10 3.33 Beck et al., 2017
260 HAdV2 4 122 30.50 Beck et al., 2017
260 MS2 2 30.3 15.15 Beck et al., 2017
265 B. subtilis 4 28 7.00 Oguma Kumiko, 2018
265 E. coli IFO 3301 4 6 1.50 Oguma Kumiko, 2018
265 Qβ 4 39 9.75 Oguma Kumiko, 2018
266 MS2 7 9 1.29 Kim Do-Kyun et al., 2017
266 Qβ 7 9 1.29 Kim Do-Kyun et al., 2017
266 ΦX174 7 1 0.14 Kim Do-Kyun et al., 2017
275 E. coli 3.8 9 2.37 Bowker et al., 2011
275 MS2 2.1 60 28.57 Bowker et al., 2011
275 T7 4.7 20 4.26 Bowker et al., 2011
280 B. subtilis 4 48 12.00 Oguma Kumiko, 2018
280 E. coli 4 13.8 3.45 Oguma Kumiko et al., 2013
280 E. coli K12(ATCC 29425) 3 9 3.00 Beck et al., 2017
280 HAdV2 4 89 22.25 Beck et al., 2017
280 MS2 2 38.5 19.25 Beck et al., 2017
280 Qβ 1 13.3 13.30 Oguma Kumiko et al., 2015
280 Qβ 4 75 18.75 Oguma Kumiko, 2018
280 ΦX174 3.2 8.9 2.78 Aoyagi et al., 2011
LP B. subtilis 4 58 14.50 Oguma Kumiko, 2018
LP E. coli IFO 3301 4 7.5 1.88 Oguma Kumiko, 2018
LP E. coli K12(ATCC 29425) 3 11 3.67 Beck et al., 2017
LP HAdV2 3 63 21.00 Beck et al., 2017
LP HAdV2 4 112 28.00 Beck et al., 2017
LP MS2 4 64.4 16.10 Roberto et al., 2014
LP MS2 2 35 17.50 Beck et al., 2017
LP T1 4 19.3 4.83 Roberto et al., 2014

2014; Beck et al., 2017 and Oguma and Surapong, 2018). In summary, specified volume of water (Oguma and Surapong, 2018), and it can be
according to the UV dose response for per log inactivation in the same calculated by Eq. (2) (Sharpless and Linden, 2005):
wavelength, inactivation capacities can be compared as follows:
ΦX174 N E. coli N T type bacteriophage N B. subtilis N MS2 or Qβ A
EEO ¼ ð2Þ
N HAdV. After discerning the inactivation capacities of different micro- 3:6  103  V  K  C  WF
organisms and the most effective wavelength, experimental model, or
amount of UV dose, scholars also conducted considerable relevant where EEO is the electrical energy per order of magnitude (kWh/m3/
research. order), A is the irradiant surface area (cm2), V is the volume of sample
We also observed the correlation of UV dose and wavelength. A chip (mL), K is the fluence-based inactivation rate constant (cm2/mJ), WF
with a short wavelength is difficult to develop and costly but features is the water factor accounting for the UV absorbance and water depth,
low optical efficiency. Owing to their high Al content and significantly and the value of 3.6∗103 is a unit conversion constant for mW and kW,
lower quantum efficiency, UV-LEDs with short wavelengths are sub- s and h, and mL and m3; and C is the wall plug efficiency which can be
stantially more difficult to fabricate than UV-LEDs with longer wave- calculated by Eq. (3) (Oguma and Surapong, 2018):
lengths; furthermore, UV-LEDs with lower quantum efficiencies
Poutput FA
produce lower optical power outputs than those generated by UV- C¼ ¼ ð3Þ
Pinput IA  VA
LEDs with longer wavelengths at the same drive current (Aoyagi et al.,
2011). Hence, encapsulation modules, which consist of short-
where Poutput refers to the UV-LED optical power (mW), Pinput denotes
wavelength chips, possess a low radiation power (radiant flux). UV
the applied electrical power (mW), IA represents the applied current
dose is directly related to radiant flux and is thus also related to the
(mA), VA corresponds to the applied voltage (V), and FA is the radiant
wavelength value. Therefore, the influence of UV dose must be analyzed
flux (mW) information provided by the manufacturer.
in combination with wavelength to analyze the least energy consuming
The UV dose (mJ/cm2) required for obtaining n-log reduction, that is,
and more promising wavelengths and the bactericidal effect of UV dose
the electrical energy per specific n-log 10 reduction, EE.n (kWh/m3/n-log
under different wavelengths. According to relevant studies and discus-
reduction), is defined in Eq. (4) (Beck et al., 2017):
sions, the best wavelengths are those at 260 and 280 nm, which feature
the highest efficiency and lowest energy consumption or electrical A  Fn
energy. EE:n ¼ ð4Þ
3:6  103  V  C  WF
The electrical energy per order, EEO (kWh/m3), is a parameter based
on electrical energy consumption, which has been used to assess the where Fn is the fluence required for n-log 10 reduction (mJ/cm2).
performance of different UV disinfection systems (i.e., UV-LEDs and Beck et al. (2017) calculated the EE.3 value for E. coli inactivation at
LPUV). EEO is defined as the amount of electrical energy required to re- 280 nm and observed a lower value (1.04 kWh/m3) compared with
duce the concentration of microbes by an order of magnitude in a that at 260 nm (1.392 kWh/m3); the EE,2 values observed for HAdV2
1422 X. Li et al. / Science of the Total Environment 659 (2019) 1415–1427

inactivation at 280 and 260 nm measured 4.401 and 5.143 kWh/m3, re- Table 2
spectively. Oguma and Surapong (2018) observed that the EE,3 values at UV dose required to achieve 4 log inactivation.

280 nm UV-LEDs were lower than those at 265 nm as the difference in Microorganism Wavelength UV dose Reference
wall plug efficiency consumed approximately half as much energy as (nm) (mJ/cm2)
265 nm UV-LEDs for all microorganisms; they also discovered that the B. subtilis 265 28 Oguma Kumiko, 2018
EE.3 values of all tested microorganisms at 300 nm were the highest E. coli K12 IFO3301 265 16.4 Oguma Kumiko et al.,
among the wavelengths, as proven by the highest wall plug efficiency 2013
E. coli K12 IFO3301 265 10.8 Oguma Kumiko et al.,
at 300 nm in the tested UV-LEDs. In brief, the 280 nm UV-LED is an op-
2013
timum choice to achieve high inactivation efficiency in low-energy- E. coli K12 IFO3301 265 6 Oguma Kumiko, 2018
consumption conditions. L. pneumophila 265 4.5 Oguma Kumiko, 2018
The change in experimental models is also connected with UV dose. Qβ 265 39 Oguma Kumiko, 2018
To achieve 4 log inactivation, researchers created a set of experimental B. subtilis 280 48 Oguma Kumiko, 2018
E. coli K12 IFO3301 280 25.5 Oguma Kumiko et al.,
models of batch and flow-through reactors. The batch reactor contained 2013
an array of nine UV-LEDs on the surface of a sample placed in a sterilized E. coli K12 IFO3301 280 13.8 Oguma Kumiko et al.,
Petri dish, whereas the flow-through reactor contained connection 2013
tubes, a sampling port, and the UV-LED cylinder, which was protected E. coli K12 IFO3301 280 9 Oguma Kumiko, 2018
HAdV2 280 89 Beck et al., 2017
by a quartz sleeve and placed in the center. The UV-LEDs with 265 nm
L. pneumophila 280 9 Oguma Kumiko, 2018
wavelength must be adjusted to fluence values of 10.8 and P. aeruginosa 280 8.5 Oguma Kumiko, 2018
16.4 mJ/cm2, but those with 280 nm wavelength must be adjusted to Qβ 280 75 Oguma Kumiko, 2018
fluences of 13.8 and 25.5 mJ/cm2 in the batch and flow-through reac- B. subtilis LP 58 Oguma Kumiko, 2018
tors, respectively (Oguma et al., 2013). Different UV doses are required E. coli K12 IFO3301 LP 7.5 Oguma Kumiko, 2018
HAdV2 LP 112 Beck et al., 2017
for different experimental model settings at the same wavelength. A
L. pneumophila LP 6.5 Oguma Kumiko, 2018
predictive model equation was designed to evaluate the viral inactiva- P. aeruginosa LP 9 Oguma Kumiko, 2018
tion effect; this equation can calculate the specific irradiation UV dose T1 LP 19.3 Roberto et al., 2014
for accomplishing the expected inactivation levels in water treatment PRD1 LP 36 Roberto et al., 2014
PhiX174 LP 8.9 Roberto et al., 2014
facilities (Kim et al., 2017). The experimental model of flow reactor
MS2 LP 64.4 Roberto et al., 2014
yields better predictions; as the flux or UV dose increases, the flow
model for decentralized and mobile water disinfection systems will pro-
duce higher inactivation, improve light output, and reduce costs in the 2018; Beck et al., 2017; Rodriguez et al., 2014). Thus, UV dose can be
form of mobile water disinfection systems in the future (Würtele used as the reference value for disinfection of drinking water.
et al., 2011). Analysis of inactivation rate constant for each microorganism in dif-
Overall, the amount of UV dose that can achieve an optimum disin- ferent wavelengths shows that a higher inactivation rate constant
fection effect must be determined, thus requiring extensive (K) (cm2/mJ) indicates an increased UV sensitivity of microorganisms
investigations. to a specific wavelength. The inactivation rate constant (K) provides a
direction for selecting the appropriate wavelength during disinfection.
3.1.3. Inactivation rate constant (K) Table 3 shows the wide variation in the inactivation rate constants of
The inactivation rate constant (K) (cm2/mJ) is equal to the sensitiv- the same species at different wavelengths. HAdV2 is a highly resistant
ity of microorganisms to UV light. First, inactivation of different micro- virus. The UV-LED wavelength of 260 nm yields the highest inactivation
organisms must be perceived at different doses; according to rate constant (K) (0.045 cm2/mJ) among 260, 280, and 260 + 280 nm
international standards, disinfection of drinking water should achieve UV-LEDs or LP; for UV-LEDs with a coupling wavelength of 260
a 4 log inactivation to reach safe levels; thus, the amount of UV dose + 280 nm, the value of inactivation rate constant (K) lies between
that can achieve 4 log inactivation will be determined (USEPA, 2006). 260 nm to 280 nm (Beck et al., 2017). For B. pumilus, the coupling wave-
Table 2 shows the required UV dose to achieve 4 log inactivation for length of 260 + 280 nm and the wavelength at 260 nm similarly yield a
the listed microorganisms in three wavelengths. The next step focuses high inactivation rate constant (K) (0.012 cm2/mJ) (Beck et al., 2017).
on qualitative analysis and comparison of the capacities for microbial in- The 265 nm wavelength yields the highest inactivation rate constant
activation. Table 2 shows that the UV-LED with 265 nm wavelength is (K) (0.174 cm2/mJ) for B. subtilis under 265 and 280 nm and LP
used to achieve adjusted fluence values of 10.8 and 16.4 mJ/cm2 for (Oguma and Surapong, 2018). The inactivation rate constant (K) of P.
over 4 log inactivation of E. coli K12 IFO 3301, but the UV-LED emission aeruginosa and Qβ in UV-LEDs emitting at 265 nm reach 0.774 and
wavelength at 280 nm is needed for the adjusted doses of 13.8 and 0.098 cm2/mJ, respectively, which are higher than that at longer wave-
25.5 mJ/cm2 in the batch and flow-through reactors, respectively lengths (Oguma and Surapong, 2018; Oguma et al., 2016). The highest
(Oguma et al., 2013). However, a large difference was noted in the UV inactivation rate constant (K) of MS2 equals 0.066 cm2/mJ in UV-LEDs
doses for E. coli K12 IFO 3301 (Oguma and Surapong, 2018); the re- emitting at 260 nm, whereas that of the coupling wavelength (260
quired inactivation UV dose, featuring a certain advantage, is 6 mJ/cm2 + 280 nm) totals 0.61 cm2/mJ (Beck et al., 2017; Oguma et al., 2016;
at 265 nm and 9 mJ/cm2 in 280 nm compared with the values of Rattanakul et al., 2014). For the most common bacteria, different E.
10.8 mJ/cm2 at 265 nm and 13.8 mJ/cm2 at 280 nm in previous batch coli strains show differences regarding the inactivation rate constant
types; the results depended on the different designs of UV-LED light (K) (cm2/mJ). Table 3 shows that the highest inactivation rate constant
source systems or water reactor systems (Oguma et al., 2013). In this ar- (K) of E. coli CGMCC 1.3373 reaches 0.41 cm2/mJ at 265 nm wavelength,
ticle, we can determine the amount of UV dose that can achieve 4 log in- whereas the second highest inactivation rate constant (K) is
activation in different microorganisms: for B. subtilis, 28 mJ/cm2 at 0.36 cm2/mJ at the coupling wavelength of 265 + 280 nm (50%) (Li
265 nm, 48 mJ/cm2 at 280 nm, and 58 mJ/cm2 under LP; Qβ, et al., 2017); however, in another study, E. coli K12 IFO 3301 yielded a
39 mJ/cm2 at 265 nm and 75 mJ/cm2 at 280 nm; L. pneumophila, high inactivation rate constant (K) of 0.805 cm2/mJ at the wavelength
4.5 mJ/cm2 at 265 nm, 9 mJ/cm2 at 280 nm, and 6.5 mJ/cm2 under LP of 265 nm and 0.811 cm2/mJ under LP lamps (Oguma and Surapong,
(Oguma and Surapong, 2018). We can also determine the UV dose for 2018). These results are primarily attributed to the different internal
maximum inactivation of HAdV2. Table 2 shows the order of the ability structures of E. coli CGMCC 1.3373 and E. coli K12 IFO 3301. The UV
of microorganisms to be inactivated by UV light: L. pneumophila N E. coli dose and logarithmic inactivation in the inactivation fitting curve can
N B. subtilis N Qβ N HAdV2 (Oguma et al., 2013; Oguma and Surapong, be also analyzed as follows: a long “shoulder” indicates aggregation of
X. Li et al. / Science of the Total Environment 659 (2019) 1415–1427 1423

Table 3 irradiation time of 300 s, they obtained a 2.7 logarithmic inactivation


Inactivation rate constant (K) (cm2/mJ) of different microorganisms. at the UV dose of 17.5 mJ/cm2 for the 269 nm UV-LEDs and a 3.7 loga-
Microorganism Wavelength K Reference rithmic inactivation at the UV dose of 34.5 mJ/cm2 for the 282 nm UV-
(nm) (cm2/mJ) LEDs; therefore, the 282 nm UV-LEDs performed significantly better
HAdV2 DNA 260 0.045 Beck et al., 2017 than the 269 nm UV-LEDs under the same time span and input power
HAdV2 DNA 260 + 280 0.049 Beck et al., 2017 owing to the higher photon efficiency of the 282 nm UV-LEDs. Aoyagi
HAdV2 DNA 280 0.032 Beck et al., 2017 previously showed that UV-LEDs with wavelengths of ~280 nm were
HAdV5 285 0.023 Oguma Kumiko et al. 2016
considerably easier to fabricate than those with wavelengths of
HAdV5 LP 0.020 Rattanakul et al., 2014
B. pumilus 260 0.012 Beck et al., 2017 ~255 nm given the lower Al content and much higher quantum effi-
B. pumilus 260 + 280 0.012 Beck et al., 2017 ciency of 280 nm UV-LEDs; thus, the 280 nm UV-LEDs yield a higher op-
B. pumilus 280 0.008 Beck et al., 2017 tical power output than the 255 nm UV-LEDs at the same drive current;
B. pumilus LP 0.010 Beck et al., 2017 the 280 nm UV-LEDs were also more effective in the actual inactivation
B. subtilis 265 0.174 Oguma Kumiko, 2018
B. subtilis 280 0.104 Oguma Kumiko, 2018
experiment owing to their higher optical power output; therefore, the
B. subtilis LP 0.099 Oguma Kumiko, 2018 use of 282 nm UV-LEDs is preferable for the overall performance of
E.coli K12(ATCC 260 0.290 Beck et al., 2017 the UV purification module (Aoyagi et al., 2011; Würtele et al., 2011).
29425) The UV-induced damage of 280 nm UV-LEDs may inhibit reactiva-
E.coli K12(ATCC 280 0.310 Beck et al., 2017
tion, thus impairing protein activities, whereas less repaired damage is
29425)
E.coli K12(ATCC LP 0.270 Beck et al., 2017 detected by endonuclease sensitive site assay. The 260 nm wavelength
29425) chip with an increased output power will result in increased inactiva-
E.coli K12 IFO3301 265 0.805 Oguma Kumiko, 2018 tion efficiency. As a result, the 280 nm wavelength remains more effec-
E.coli K12 IFO3301 280 0.561 Oguma Kumiko, 2018 tive and relatively cheap, but by the progress in the UV-LED chip R&D
E.coli K12 IFO3301 LP 0.811 Oguma Kumiko, 2018
technology, the ~260 nm wavelength chips may feature a more compet-
E.coli CGMCC 1.3373 265 0.410 Guo-Qiang Li et al., 2017
E.coli CGMCC 1.3373 260 + 280 0.360 Guo-Qiang Li et al., 2017 itive wavelength range of light in the future.
(50%)
E.coli CGMCC 1.3373 260 + 280 0.320 Guo-Qiang Li et al., 2017 3.2. Influence of UV-LED light source on water treatment system settings
(75%)
E.coli CGMCC 1.3373 280 0.300 Guo-Qiang Li et al., 2017
E.coli CGMCC 1.3373 LP 0.350 Guo-Qiang Li et al., 2017 UV-LED light source is applied in water to sterilize microorganisms.
MS2 260 0.066 Beck et al., 2017 The settings of water treatment system significantly influence the mi-
MS2 260 + 280 0.061 Beck et al., 2017 crobial disinfection effect. This kind of reaction environment will di-
MS2 280 0.052 Beck et al., 2017 rectly influence the “quality” and “quantity” of receiving UV-LED light
MS2 285 0.029 Oguma Kumiko et al.,
source, thereby affecting the microbial inactivation effect. To maximize
2016
MS2 LP 0.056 Beck et al., 2017 the effect of UV-LED light source systems, changes should be made in
MS2 LP 0.041 Rattanakul et al., 2014 the water treatment system. This section mainly focuses on the follow-
P. aeruginosa 265 0.774 Oguma Kumiko, 2018 ing aspects: the working mode of water sample, water treatment reac-
P. aeruginosa 280 0.511 Oguma Kumiko, 2018
tors, and the influence of auxiliary equipment on inactivation.
P. aeruginosa LP 0.448 Oguma Kumiko, 2018
Qβ 265 0.098 Oguma Kumiko, 2018
Qβ 280 0.056 Oguma Kumiko, 2018 3.2.1. Working mode of water sample
Qβ 285 0.037 Oguma Kumiko et al., The design of the reactor is a key factor according to experimental
2016 analysis; it directly affects the result of the water treatment system
Qβ LP 0.085 Oguma Kumiko, 2018
and is directly related to the working mode of experimental models.
To date, a simple reactor is most commonly used to perform a series
of experiments on variation parameters, and it occasionally achieves
microorganisms and damage regeneration. “Tailing” mainly occurs in the aim of studies by changing the structure and parameter from a UV
resistant species, including those with adaptive resistance. Different transmitter. Most scholars also use novel methods of working modes,
strains under each wavelength exhibit different inactivation rate con- such as batch type and flow-through reactors, to change the state of mi-
stant (K), but E. coli is the most sensitive; on the other hand, bacterio- crobes and further discuss their properties. New discoveries are
phage Qβ and B. subtilis spores are more resistant compared with achieved using these experimental models.
other bacteria (Oguma and Surapong, 2018). These microorganisms be- Several scholars compared the sensitivities of bacteriophages MS2,
longing to different species possess varying internal structures, Qβ, and ΦX 174 by the experimental models of batch type and flow-
resulting in different experimental results. through reactors. In the batch type reactor, the UV-LEDs with 266 nm
Based on the overall analysis, the sensitivity at ~260 nm is generally wavelength were used for irradiation. Then, over 7 log reductions of
better than that at ~280 nm. However, in the current conditions, the UV- 9 mJ/cm2 for MS2 and Qβ and 1 mJ/cm2 for ΦX 174 were observed dur-
LED chips emitting at 260 nm incur considerably high production costs ing exposure. Scholars also observed the similar inactivation rate con-
due to the considerable difficulties in R&D, whereas the optical intensity stants of MS2 and Qβ, whereas ΦX 174 was the most sensitive to
and external quantum output lack strength. On the other hand, the UV- 279 nm UV-LEDs, LP, or the other experiments by a flow-through reac-
LED with 280 nm wavelength is more effective in actual inactivation ex- tor (Kim et al., 2017). These experimental results are consistent with
periments as the 280 nm wavelength yields more external output and those of other studies on ssDNA virus ΦX 174 or ssRNA viruses MS2
emits light with high efficiency. For example, Lawal et al. (2018) ob- and Qβ; the UV sensitivities of viruses have been evaluated by the inac-
served that the external quantum efficiency of an UV-LED reached tivation rate constant (K) (cm2/mJ), and statistically higher UV sensitiv-
0.01%–4.5% and 0.1%–20.5% at ~255 and ~280 nm, respectively. That is, ity and inactivation rate constant were observed in ΦX 174 than in other
the external quantum efficiency of 280 nm UV-LEDs was almost 5–10 viruses; these results coincide with the findings of other research that
times that of 255 nm UV-LEDs, and although the disinfection efficiency studied the three viruses by UV (Hijnen et al., 2006; Aoyagi et al.,
at 255 mm was twice that at 280 nm, the total disinfection efficiency of 2011). The 269 nm wavelength is close to the maximum absorption
the UV-LEDs operating at 280 nm was nearly five times larger (Aoyagi peak of B. subtilis spores and may present better germicidal effective-
et al., 2011; Lawal et al., 2018). When Würtele et al. (2011) studied B. ness than 282 nm UV-LEDs. However, a different condition was ob-
subtilis spore inactivation by UV-LED at the same input power and served when 269 and 282 nm UV-LEDs utilized the same input power
1424 X. Li et al. / Science of the Total Environment 659 (2019) 1415–1427

and exposure time. These conditions resulted in different fluence values. inactivated by static reactors, achieving an excellent inactivation effect.
Static and flow-through tests are experimental methods designed for The radiation distance from UV transmitter to static reactor should be
analysis. The flow-through test first indicates a linear correlation rela- kept a close range and carefully consider the microbial receiving radiant
tionship between inactivation and fluence and demonstrates a well- flux. This procedure increases the number of UV-LED to achieve a better
designed flow-through reactor; owing to their higher photon output, disinfection effect, such as that shown Fig. 3, where the reactor can use
the 282 nm UV-LEDs caused a significantly better inactivation of B. an array of nine UV-LED chips or more for light emission to improve the
subtilis spore than the 269 nm UV-LEDs at the same time range and inactivation efficiency.
input power (Chen et al., 2009); however, in flow-through tests, the in- By contrast, flow-through reactors are more complex and include di-
activation rate constant (K) of B. subtilis spores was more than halved verse models, which also depend on the application environment.
compared with that in static tests, whereas the inactivation of B. subtilis Würtele et al. (2011) designed a reactor system in which the test
was also reduced (Würtele et al., 2011). These results are attributed to water flows from the feed reservoir through the flow-through reactor
the tailing phenomenon in the flow-type reactor, as shown in the and accumulates in the catchment tank. Other researchers designed a
fluence–response curves, resulting in lower inactivation efficiency hollow chamber, through which the water sample can pass freely,
than that in the batch reactor, which yielded a lower fluence-based in- surrounded with multiple chips, pumps, or reservoirs added to acceler-
activation rate constant of 29% in 265 nm and 32% in 280 nm wave- ate the water cycle (Aoyagi et al., 2011; Kim et al., 2017). This reactor
length (Oguma et al., 2013); tailing may originate from the design for water flow features dependency on pressure and a hardly
aggregation of microorganisms and can cause spore aggregation, controllable temperature; the irradiation may also be insufficient of
which was observed by scanning electron microscopy of the aggregate deep UV light when certain amount of water passes through the cham-
size in relation to the 3 ml polycarbonate filter pores (Mamane and ber. Thus, sufficient irradiation must be guaranteed. If the dosages nec-
Linden, 2005; Mattle and Kohn, 2012); the flow-type reactor requires essary for 3 to 5 log reduction were calculated, the flow and circulating
a longer operation time than the batch reactor, providing higher possi- disinfection system can be used to accomplish higher reduction of
bility for microbial aggregation. In a flow-type reactor, UV-LEDs with Human Enteric Viruses, and the proper UVC-LED treatment level for
different coupling peak emissions are less effective than those used sustaining potable water safety can be determined from the data. An-
alone and reduce the output power for each UV-LED (Oguma et al., other research team fabricated a water reactor made of two quartz
2013). UV-LEDs showed higher-time-based inactivation efficiency sleeves according to the principle of the connected device, and the UV
with peak emission at 280 nm owing to the highest output power transmitter comprised three arrays that were bundled to build an equi-
achieved at this wavelength compared with that at 265 or 310 nm; lateral triangular prism, which was placed in a quartz sleeve and
meanwhile, UV-LEDs achieved the highest fluence-based efficiency at inserted in the center of a cylinder (Oguma et al., 2013). This
265 nm because of the highest UV absorbance of DNA at this wave- connector-type reactor design is more convenient to clean than other
length (Jagger, 1967). Most UV reactors are used by flow-through reac- flow designs given the flexible detachability. Several researchers de-
tors but not static reactors, as fluence is linearly associated with signed a disinfection system and placed the UV-LED lamp next to the
inactivation in flow-through reactors. Flow-through reactors can also quartz tube to be used in combination with the ultrasound module;
accelerate water cycle treatment; hence, UV-LEDs are applied in water this design may be suitable for small-household water-disinfection
disinfection systems under flow-through reactors to minimize tailing equipment (Andrej et al., 2015). In summary, flow-through reactor
and improve efficiency (Würtele et al., 2011; Oguma et al., 2013). should maintain a sufficient irradiation in the chamber where water
The above conditions can be changed in experimental modes of dif- would flow (Fig. 4). This design is also a good way to set additional
ferent reactors, and other aspects, including improvements of materials UV-LEDs chips array around the chamber or extend the chamber length,
in the reactors, can be discussed. For instance, quartz glass reactors can allowing the water to receive sufficient UV light.
be used as light guides that use total emission to further improve disin- At present, although different reactor designs could significantly af-
fection (Andrej et al., 2015). fect inactivation efficiency, the disinfection effect of different water re-
actors is difficult to define accurately given the presence of numerous
3.2.2. Water treatment reactors environmental factors. The disinfection effects of different reactors
Water treatment reactors generally include two forms: static and may be defined using experimental models, such as static and flow-
flow-through reactors. Different reactor designs exert varying effects through reactors (the latter performs better, as mentioned). In other
on inactivation efficiency, as mentioned in the previous section. In this words, more benefits and multiform design reactors can still be
section, we will discuss the reactor designs that significantly affect inac-
tivation efficiency and have been reported in literature. A reactor is gen-
erally related to the UV transmitter and application environment.
In general, static reactors use a deep or shallow petri dish with an ei-
ther long or short radius. A stirrer is also necessary and is set up at the
bottom or suspended midair in the reactor. The stirrer can accelerate
the uniformity of water, allowing the UV transmitter to fully disinfect
water samples. Several researchers used a petri dish equipped with a
suspended agitator and was placed on the top of the UV LED array for
static tests (Würtele et al., 2011). Others created a ring-shaped UVC-
LED apparatus attached to the outer rim of a fused silica quartz dish
for disinfection (Oguma et al., 2016). However, possibly focusing more
on the UV transmitter than the static reactor, most researchers followed
the experimental requirements and designed a simple and suitably
sized static reactor with a magnetic stirrer at the bottom and a UV trans-
mitter equipped with a multiple-chip array on the top (Oguma et al.,
2013; Chevremont et al., 2012b; Akgün and Ünlütürk, 2017; Li et al.,
2017). The static reactor features a better aim at microorganisms, as
water exhibits small vibration and no large flow. Thus, the static reactor
is suitable for the inactivation of microorganisms with strong UV resis-
tance. Notably, the microorganisms with weak anti-UV ability are also Fig. 3. Optimized static reactor design (Oguma et al., 2016).
X. Li et al. / Science of the Total Environment 659 (2019) 1415–1427 1425

explored and improved. On the other hand, the application of static and One group proposed a new purification system combining UV-LED
flow-through reactors becomes more practical in life. For example, with solar cells; these nested auxiliary modules are innovative and use-
static reactors can be made with small UV-LED embedded device for ful in solving the power supply of UV-LED disinfection systems (Aoyagi
air surface or shallow liquid disinfection, especially for the disinfection et al., 2011). The mature and widely used auxiliary equipment adds an
of small medical instruments, such as stethoscope membranes and sur- ultrasound treatment unit to improve the bactericidal effect.
gical tools, or personal belongings and household articles, such as con- DOM is ubiquitous in natural waters, and 90% of DOM includes
tact lenses, toothbrush, tableware, baby bottles, and toys; flow humic substances that can be divided into hydrophobic (humic acids)
reactors can be used for flow water disinfection in water dispensers, and hydrophilic (fulvic acids) components (Barber et al., 2001;
water purifiers, and washing machines. Thurman, 1985; Thurman and Malcolm, 1981); these substances can
absorb UV (Liu et al., 2018). Humic acid was also discovered to display
3.2.3. Auxiliary system affinity for various surfaces, and its addition to water samples can coat
After ensuring the setup for the UV transmitter and reactor, we can bacteria to absorb UV and reduce the sensitivity of cells to UV light
still add an external auxiliary equipment to further improve the disin- (Cantwell et al., 2008; Vilhunen et al., 2009). Thus, reducing the influ-
fection efficiency. The final problem is to solve the radiation problem ence of DOM is another major challenge in water treatment systems.
of microorganisms in water or enhance the convenience of the overall Coagulation–ultrafiltration processes, such as those involving alumi-
system. First, we should focus on key factors, such as water turbidity num sulfate, ferric chloride, and polyaluminum chloride, can effectively
or dissolved organic matter (DOM), which affect water quality and remove DOM (Chow et al., 2009; Hu et al., 2018; Bu et al., 2018; Yang
weaken UV radiation. et al., 2007).
When the water sample is turbid and contains particles, the reflec- A multiple filtration system or coagulation–ultrafiltration system
tion of particles in the water sample will reduce the UV radiation or pos- should be embedded in the front-end systems using turbid water or
sibly cause the accumulation of microorganisms (Blume and Neis, water containing DOM as sample. Other auxiliary equipment that fur-
2004). Thus, water treatment designs must maximize the UV dose to ther improves UV disinfection efficiency and still awaits discovery and
ensure that pathogens are adequately exposed to UV radiation and to ef- exploration.
fectively reduce pathogenic bacteria to a level safe for human consump-
tion (Nelson et al., 2012). The low turbidity will also shelter 4. Conclusion
microorganisms and can change the UV transmittance of water and re-
duce UV radiation on target microorganisms. Consequently, by adding UV-LED water disinfection systems cover a wide range of topics.
water pretreatment designs to improve radiation from UV transmitters These systems include not only the microelectronics packaging technol-
or exposing more water sample to radiation, we can combine several ogy of UV-LED chips or module design but also the inactivation of path-
LEDs to irradiate a small volume of water, which is agitated during the ogens in water-environment engineering analysis. This subject requires
entire treatment time (Nelson et al., 2012). Early in 2009, Gibson technical personnel with mastery of comprehensive knowledge to per-
discussed the effect of suspension particles on urban waste water and form analysis from various perspectives. This article is based on the
demonstrated that low-frequency ultrasound can break down bacterial comprehensive analysis and investigation of various wavelengths of
flora (Gibson et al., 2009). The main principle applied on the ultrasound disinfection and energy consumption of UV-LEDs and problems en-
unit is that low-power consumption in the UV-LED disinfection system countered in the water treatment process. Several constructive conclu-
suits implementation and can achieve acoustic cavitation, thereby cre- sions are drawn for reference purposes.
ating a purification effect and achieving synergistic effects with UVC ra- With regard to the investigation of the inactivation efficiency and
diation within the disinfection system (Jin et al., 2013). This ultrasound energy consumption of UV-LEDs for pathogens at various wavelengths,
pretreatment can achieve the effect of mechanical shear force and con- selecting a wavelength and setting a system that matches high-
sequently change the particle size distribution as reported in previous efficiency UV-LED water disinfection equipment will benefit future
studies (Zhou et al., 2017). For instance, several research were con- studies. Future UV-LED water treatment designs should add a pretreat-
ducted on the use of ultrasound-enhanced UV disinfection technology ment process in high-turbidity water to reduce interference in the early
with combined theoretical and experimental bases. The generation of stage (Nelson et al., 2012). UV dose is a key parameter in evaluating the
transient cavitation was demonstrated by disintegrating aluminum effects of disinfection; it benefits from the integrated calculation of radi-
foil and adding multiple ultrasonic probes around a mercury lamp to ant flux, exposure time, and attenuation factors, among which attenua-
improve the efficiency of UV disinfection (Andrej et al., 2014; Bazyar tion factors, including water factor, reflection factor, divergence factor,
et al., 2013). Given its powerful effect, ultrasound pretreatment treat- and sensor factor, are particularly complex (Bolton and Linden, 2003);
ment is also a feasible method to improve UV disinfection efficiency. the improvement of water treatment systems will be accompanied by

Fig. 4. Optimized flow-through reactor design (Aoyagi et al., 2011).


1426 X. Li et al. / Science of the Total Environment 659 (2019) 1415–1427

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