Journal of Petroleum Science and Engineering 22 Ž1999.

121–130

Advances in hydrocarbon generation theory žI /

Generation and evolution model for immature oils and
hydrocarbon
)
Difan Huang
Research Institute of Petroleum Exploration and DeÕelopment, CNPC, P.O. Box 910, Beijing 100083, China

Abstract

The wide existence of immature oils throughout the world, especially in China, broke through the hydrocarbon generation
theory of kerogen thermal degradation. Studies have shown that soluble and insoluble organic matter are organically
connected in the sedimentary rock, both contributing to hydrocarbon generation. In the diagenesis, kerogen cannot produce
oils, so immature oils derive directly from the degradation of the soluble lipids. Hydrocarbon generation process by kerogen
thermal degradation takes place mainly in the early catagenesis Ž R o s 0.5–1.2%., and the oils generated are normal. In the
late catagenesis, hydrocarbon generation comes into wet gas stage Ž R o s 1.2–2.0%., with pyrobitumen and oils cracking
into high mature light oils and wet gases, respectively. In this paper, the author presented a novel general model of
hydrocarbon generation and evolution with soluble and insoluble organic matter both contributing to hydrocarbon
generation. q 1999 Elsevier Science B.V. All rights reserved.

Keywords: Immature oils; Kerogen; Soluble organic matter; Generating hydrocarbon and evolution

1. Hydrocarbon generation theory of kerogen
thermal degradation and immature oil
Hydrocarbon generation theory of kerogen ther-
mal degradation was gradually developed in the late
1960’s ŽLouis, 1964; Philppi, 1965; Mclver, 1967;
Louis and Tissot, 1967; Albrecht and Ourission,
1969; Vassoevich and Akramkhodzhaev, 1974.. The
theory was discussed systematically and scientifi-
cally in two excellent works by Tissot and Welte
Ž1978., Hunt Ž1979. and Tissot and Welte Ž1984. .
During the last fifteen years, studies on petroleum
origin stepped out of basic studies and developed
)
Tel.: q86-10-62098443; Fax: q86-10-62017181; E-mail:
georiped@public.bta.net.cn
toward applied technique field, becoming a very
effective and highly applicable technique in
petroleum exploration with the foundation of the
hydrocarbon generation theory of kerogen thermal
degradation.
The elementary thoughts of this theory are cited
as follows. At the end of diagenesis, the organic
matter consists mainly of kerogen. Thermal degrada-
tion of kerogen is responsible for the generation of
most hydrocarbons, i.e., oil and gas. Kerogen is the
main precursor of petroleum compounds ŽTissot and
Welte, 1978.. A sedimentary rock must pass though
the time–temperature threshold of intense hydrocar-
bon generation in order to form enough hydrocar-
bons to yield commercial petroleum accumulations.
The rate of hydrocarbon generation from kerogen

0920-4105r99r$ - see front matter q 1999 Elsevier Science B.V. All rights reserved.
PII: S 0 9 2 0 - 4 1 0 5 Ž 9 8 . 0 0 0 6 1 - 8
122 D. Huangr Journal of Petroleum Science and Engineering 22 (1999) 121–130
increases exponentially with a linear increase in tem-
perature. The quantity of oils and gases formed
depends primarily on the kerogen type, temperature
and time ŽHunt, 1979.. From this theory, geo-
chemists established a series of highly applicable
geochemical parameters and research methods deal-
ing with evaluation hydrocarbon potential. These
parameters and research methods can be summarized
as the following aspects: division of hydrocarbon
generation and evolution stages; determination of
upper and lower threshold values; judgment of hy-
drocarbon origin and origin analysis by biomarker
assemblage; determination of three factors affecting
hydrocarbon generation potential Žsedimentary or-
ganic matter abundance, type and maturity.; estab-
lishment of hydrocarbon generation model of kero-
gen thermal degradation and the comprehensive
analysis and numerical modeling of sedimentary his-
tory, thermal history and hydrocarbon generation and
evolution history ŽLopatin, 1969; Tissot, 1969;
Lopatin, 1971; Hood et al., 1975., etc. With these
parameters and methods, remarkable achievements
have been made. They also become the principles for
petroleum exploration.
In the early 1980’s, on the basis of this theory,
together with the abundant nonmarine hydrocarbon
and source rocks’ geochemistry materials, we sum-
marized the principles of hydrocarbon generation
and evolution systematically and defined a series of
corresponding geochemistry indexes. We also devel-
oped and perfected nonmarine hydrocarbon genera-
tion theory, making an important conclusion that the
formation of terrestrial petroleum is an unavoidable
outcome of geohistory development, lake evolution
and chemical evolution of biological kingdom ŽHuang
and Li, 1982; Huang et al., 1984..
Marked successes of this theory have been
demonstrated in oil and gas exploration. Most of the
oil and gas resources have a close relationship with
this theory. However, this theory obviously ignores
the contribution of soluble organic matter in the
sedimentary rock to hydrocarbon generation in the
diagenesis and early catagenesis. Hence, the theory
cannot give a reasonable and scientific explanation
to the formation of immature and low mature oils.
On the basis of hydrocarbon generation theory of
kerogen thermal degradation, kerogen has a loose
structure, rich in O, N, S and other heteroatoms,
generating little petroleum in the diagenesis before
the formation of fossil kerogen, i.e., the developing
period for young kerogen. Besides, in accordance
with Van Krevelen curve which reflects kerogen
element composition evolution, kerogen mainly gets
rid of heteroatomic groups, releasing CO 2 , H 2 O and
CH 4 in the process of maturation above the thresh-
old of oil generation. Therefore, the theory cannot
explain the formation of immature oils. Tissot and
Welte Ž1984. held that these immature heavy oils
contain abundant heterocompounds Žresins and as-
phaltenes. and they come from an early breakdown
of kerogen with the associated high sulfur and nitro-
gen content. This means that the origin of immature
oils still deals with kerogen degeneration. On the
contrary, we think that in the diagenesis, part of the
organic matter containing biochemically synthesized
hydrocarbons is decomposed and the rest of it will
be condensed into kerogen or directly transform into
hydrocarbons, contributing to the formation of imma-
ture oils together with the residual lipids. Therefore,
there is an evident dominance of biological configu-
ration in the immature oils.
To solve the discrepancy between hydrocarbon
generation theory of kerogen thermal degradation
and the wide existence of immature oils, Snowdon
and Powell Ž1982. proposed to modify hydrocarbon
generation model for terrestrial organic matter. Pala-
cas et al. Ž1983. studied immature–mature oils from
the Cretaceous carbonate-evaporate of lagoon facies
in the Southern Florida Basin, the United States. He
pointed out that these carbonate-related reservoirs
form more in the late diagenesis than in the catagen-
esis. Fu et al. Ž1985., based on the study on the
immature oils in salt rock sediments, held that envi-
ronment for salt rock deposition is strongly reduc-
Table 1
Relative quantity Ž%. of hydrocarbons and soluble heavy compo-
sitions in the source rocks at different evolution stage Žafter Hunt,
1979.
Evolution stage Gas Liquid Resinsq
hydrocarbons hydrocarbons asphaltenes
Diagenesis 7 9 40
Catagenesis 82 91 60
Metamorphism 11 trace trace
Estimated according to relative carbon content.
 D. Huangr Journal of Petroleum Science and Engineering 22 (1999) 121–130
Fig. 1. Generating hydrocarbon and evolutionary section of Tertiary source rock in Raoyang sag and Qianjiang sag ŽThe upper is after Liang, 1982, unpublished work; The lower
is after Jiang, 1982. The evolutionary stage is slightly modified..

123
124 D. Huangr Journal of Petroleum Science and Engineering 22 (1999) 121–130

tive, facilitating the early reservation and transforma- immature oils in the general scheme of the organic
tion of organic matter. He also thought that the matter evolution. Hunt Ž1979. introduced the typical
existence of immature oils is a challenge to hydro- immature oils from the oil pools in the caprocks of
carbon generation theory of kerogen thermal degra- salt dome and knoll existing in the Gulf of Mexico
dation. Huang and Li Ž1987. suggested, ‘‘immature and from deltas in California and Orinoco ŽBrazil..
oils directly come from the degradation of soluble He also located immature oils in organic matter
organic matter in the source rocks at low tempera- maturation and evolution figure. However, immature
ture’’. oils were located in the early diagenesis. Early gen-
eration also appear to be common for organic matter
rich in resinite, although this has been questioned.
2. Distribution of immature oils Therefore, Tissot and Hunt both noticed the exis-
tence of immature oils while elaborating and summa-
Immature oils, belonging to heavy oils and some rizing hydrocarbon generation theory of kerogen
condensates, should be defined as the oils formed in thermal degradation, but they did not carry out fur-
the late diagenesis before the evolution of organic ther researches. These examples of immature oils do
matter in the sedimentary rocks reaches the oil not seem to be in the tune with the theory itself.
threshold. Their source rocks’ vitrinite reflectances Immature oils were first reported in China in 1982
are 0.3–0.7%. Žcalled low mature oils at that time.. Jiang and
Being confined to hydrocarbon generation theory Zhang Ž1982. and Shi et al. Ž1982. reported the
of kerogen thermal degradation, in spite of the wide immature oils from Y1-18 well in Yihezhuang Oil-
existence of immature oils all over the world, people field, Shandong Province and from Guanghua Tem-
always ignore the study on the exploration and de- ple Oilfield, Jianghan depression, respectively. Soon
velopment of immature oils and their forming and after, immature oils stimulate great interests of Chi-
accumulating conditions. There is also a great differ-
ence in evaluating immature oil resource potential.
Tissot and Welte Ž1978. estimated, ‘‘Although some
accumulations of immature, nondegraded heavy oils
are known, they possibly amount to less than 1% of
the world reserves of this category’’. But if estimated
according to the relative quantity of hydrocarbons
and soluble heavy composition in the source rocks at
different hydrocarbon generating stage ŽTable 1., the
immature heavy oil resources should take up more
than 10% of the world’s total resources.
Immature and low mature oils distribute very
widely, including both China and other countries
from terrestrial facies to marine facies. Martin et al.
Ž1963. gave an example of North American imma-
ture oils in the study of normal alkanes distribution
in crude oils. Besides the examples mentioned above,
immature asphalt from organic-rich carbonate rocks
in Upper Cretaceous Senonian in Israel ŽTannen-
baum et al., 1984, 1985., and the immature conden-
sates from southeastern Mediterranean coastal plain
in Israel ŽNissenbaum et al., 1985. are also notice-
able examples. Fig. 2. Comparison between Tertiary oil and rock extract composi-
Tissot and Welte Ž1978. mentioned some imma- tion in the Liaohe Basin wafter Piao, 1984, unpublished work;
ture oil examples in the world, but did not locate the modifiedx.
 D. Huangr Journal of Petroleum Science and Engineering 22 (1999) 121–130 125

nese geochemists. In several years, immature and
low mature oils were reported in nearly every terres-
trial Mesozoic–Cenozoic hydrocarbon basins in
China ŽShi and Wang, 1985; Wang and Shi, 1986;
Zhou, 1987; Huang et al., 1987; Huang et al., 1989;
Chen and He, 1990.. At the same time, the studies
on the hydrocarbon generation precursor, generation
conditions, distribution characteristics, and formation
mechanism of immature oils are being further carried
out ŽFu et al., 1985; Qin, 1987; Huang and Li, 1987;
Huang et al., 1987; Wang et al., 1995.. Studies
demonstrate that such oils exist mainly in Tertiary
and next in Cretaceous. Moreover, salt lake facies
and brackish water facies are especially favorable for
the formation of immature oils.
3. Contribution of dispersed organic matter to
early hydrocarbon generation in sedimentary rock
For hydrocarbon generation and evolution of
kerogen, one of the important mark is the decrease of
its HrC atom ratio or S 2 peak in Rock–Eval analy-
sis, while the evolution of young kerogen in diagene-
sis before reaching the threshold of hydrocarbon
generation generally shows the increase of the above
two indexes ŽLaplante, 1974; Huang et al., 1984.. It
means that the young kerogen not only contributes
little to hydrocarbon generation but also is accumula-
tion its ‘raw material’ for hydrocarbon generation
and preparing conditions for the following hydrocar-
bon generation of thermal degradation.

Fig. 3. The relative contribution of the three kinds of organic matter in brown coal to the generation of kerogen, humic acid and
hydrocarbons at different temperatures.
126 D. Huangr Journal of Petroleum Science and Engineering 22 (1999) 121–130

The soluble organic matter in sedimentary rock in tant information on its hydrocarbon generation. All
diagenetic stage is extremely active and at a enor- profiles of hydrocarbon generation and evolution in
mously changing state, which provide us with impor- Chinese oil–gas bearing basins reflect a kind of

Fig. 4. Production rate by thermal degradation, C 21 yrC 22q, OEP and PrrPh as a function of temperature for brown coal from Nanning
basin, China Žafter Xia and Luo, 1996..
 D. Huangr Journal of Petroleum Science and Engineering 22 (1999) 121–130 127

unified model in essence, with the content of nonhy- kerogen and humic acid, respectively. However, as
drocarbon decreasing and that of hydrocarbon in- to the formation of chloroform bitumen, especially
creasing in diagenetic stage as shown in Fig. 1. In for hydrocarbons, extractable matter is the major
group composition, nonhydrocarbon in rocks gener- contributor in early period Ž270., while kerogen is
ally decreases from 70 to 50%, whereas hydrocarbon the major contributor in medium to late stage Ž350
increases from 25 to 50% or so. The cross point and 4008C..
generally represents the threshold of hydrocarbon Xia and Luo Ž1996. in the Lanzhou Institute of
generation. It is apparent that the increase of hydro- Geology, Chinese Academy of Sciences, made a
carbon is mainly derived directly from decarboxyla- successful experiment to simulate the generation of
tion of nonhydrocarbon. At the same time, part of alkane with Tertiary brown coal from the Nanning
nonhydrocarbon together with humic acid is poly- Basin. The experiment temperature ranges from 250
condensed into kerogen. Although young kerogen to 5508C, the interval of which is 50. In every
also undergoes dehydrocarboxylation and releases interval, samples are heated isothermally for 72 h.
other heteroatomic radicals in diagenetic stage, it The experiment is classified into two groups: Y and
cannot generate hydrocarbon. This is proved by the Z. The samples of group Y are heated continuously,
fact that hydrogen content of the young kerogen whereas those of group Z are heated periodically,
either maintains constant or increases slightly. All of with the products at different temperatures extracted
the above show that the change of molecular geo- and heated at a 508C higher temperature. Therefore,
chemical parameters in rock extracts, such as the group Y experiment shows the process of thermal
decrease of OEP and CPI, and the increases of EOP
Žtends to 1. all represent the evolution of soluble
organic matter and have nothing to do with kerogen
evolution. After the evolution of organic matter
passes through threshold of oil generation in early
catagenetic stage, hydrocarbon generation by kero-
gen thermal degradation continues growing and a
large amount of hydrocarbon generated from kero-
gen thermal degradation covers of dilutes the imma-
ture–low mature characteristics of hydrocarbon de-
rived from early soluble organic matter.
Ternary diagram ŽFig. 2. of oil–rock group com-
position in Xialiaohe Basin also demonstrates that
marginal low mature crude oil from Gaosheng oil
field can only be derived from the soluble organic
matter of type-in immature source rock, with nonhy-
drocarbon and asphaltenes accounting for 50%.
Some evidence may be numerated, strengthening
the above analysis on the contribution of kerogen
and soluble organic matter to hydrocarbon genera-
tion in different stages in the natural profile of
hydrocarbon generation and evolution.
Zhang et al. Ž1995. studied the interconversion of
kerogen, humic acid and extracts in brown coal and
their contribution to hydrocarbon generation at dif-
ferent temperatures by hydrous pyrolysis ŽLewan et
al., 1979; Lewan, 1983; Lewan et al., 1986.. As
shown in Fig. 3, the humic acid and extractable Fig. 5. Hydrocarbon generation and evolutionary model of organic
matter are the major contributors to the formation of matter Žafter Huang et al., 1991.
128 D. Huangr Journal of Petroleum Science and Engineering 22 (1999) 121–130
evolution of all organic matter in brown coal, and
group Z shows the thermal evolution of kerogen. As
shown in Fig. 4, the experiment clearly distinguishes
the contribution of kerogen and soluble organic mat-
ter to hydrocarbon generation. At the same time, the
differences between the geochemical characteristics
of their products are shown in Fig. 4 clearly. Fig. 4
shows the following. Ž1. The highest peaks for hy-
drocarbon generation of kerogen and soluble organic
matter occur at 350 and 4008C, respectively. Ž2. At
400, hydrocarbon generating potential for kerogen is
nearly exhausted. Therefore, nC 21 yrnC 22q reaches
its maximum at 4508C, showing the composition
feature of normal alkane in bitumen from kerogen
thermal degradation. Ž3. Normal alkanes from kero-
gen thermal degradation have no odd–even predomi-
nance. The odd–even predominance is the feature of
immature soluble organic matter. It gradually de-
creases with the adding and blending of products
from kerogen thermal evolution and disappears cor-
responding to the peak of hydrocarbon generation of
kerogen. It also means the end of hydrocarbon gener-
ation of soluble organic matter in diagenesis. Ž4.
PrrPh in the products from kerogen thermal degra-
dation is relatively higher and does not vary with the
Fig. 6. Hydrocarbon generation during the evolution of organic matter and its relationship with the origin of parent material and the property
of oil and gas.
temperature, which affects the ratio of PrrPh in
soluble organic matter in the same way. Its blending
and thermal degradation cause the original low PrrPh
in soluble organic matter to increase gradually and
reach the maximum value at 3508C. Ž5. When the
temperature is above 4008C, the lower part of every
hydrocarbon generation curve shows that PrrPh de-
creases, and C 21 yrC 22q reaches its maximum and
OEP increases slightly. All these geochemical char-
acteristics are determined by the evolution of asphalt
or pyrobitumen from kerogen degradation.
After all, as the experiment shows, soluble or-
ganic matter plays an important role in hydrocarbon
generation. Especially in immature and relatively
higher mature stages, the products of soluble organic
matter have important impact on geochemical pa-
rameters.
4. A novel general model of hydrocarbon genera-
tion and evolution
Soluble and insoluble organic matter in sedimen-
tary rock are a whole in organic relation and keep in
 D. Huangr Journal of Petroleum Science and Engineering 22 (1999) 121–130
a state of dynamic equilibrium of interconversion in
the process of hydrocarbon generation with the
changing of physico-chemical condition. In diage-
netic stage, part of soluble organic matter in rock
will be converted to immature oil, and the other part
will be condensed into kerogen. In catagenetic stage,
kerogen thermal degradation will inevitable undergo
the intermediate stage in which bitumen is formed.
Even at high level of maturity, pyrobitumen derived
from kerogen becomes the major contributor to high
mature light oil after the hydrocarbon generating
potential for kerogen getting exhausted. Hence, to
establish an objective model, organic matter in rock
must be regarded as a unity.
In order to understand the process of oil and gas
generation comprehensively, we propose the model
shown in Fig. 5 ŽHuang et al., 1991..
The model shows different paths of evolution in
gas-prone and oil-prone environments Žhumification
for gas and saprofication for oil.. It also emphases
the contribution of soluble organic matter Žincluding
humin. to hydrocarbon generation. The model shows
not only the matrix types and their different potential
for hydrocarbon generation, whether oil or gas is
predominant, but also phasic characteristics of hy-
drocarbon generation and the maturity of correspond-
ing products in different stages which include imma-
ture oil and gas. The maturation sequences of crude
oil in nonmarine hydrocarbon basin are also reflected
in the model clearly. Finally, as shown in Fig. 5, the
three hydrocarbon generation and evolution stages
have their own characteristics: heavy oil is formed at
diagenetic stage characterized by the degradation of
soluble lipid to generate hydrocarbon directly and
the formation of fossil kerogen; the earlier phase of
catagenesis Ž R o - 1.2%. is characterized by the for-
mation of normal oil predominantly derived from
kerogen thermal degradation, whose active energy is
less than 160 kJ; at the end of the earlier phase, the
potential of kerogen for hydrocarbon generation is
exhausted; the late phase of catagenesis is character-
ized by the formation of light oil and wet gas by
cracking of pyrobitumen and normal oil, respec-
tively, whose active energy is 160–200 kJrmol; dry
gas is formed in metagenesis stage. The relationships
of hydrocarbon generation, source of original matter
and nature of hydrocarbon in the evolution process
of organic matter are illustrated in Fig. 6 clearly.
129
5. Conclusion
Ž1. Immature oils are generated directly from
soluble organic matter which contain biosynthetic
hydrocarbons, different from the ‘protopetroleum’ in
Recent and Quaternary sediments. Their wide exis-
tence and economic value break through the limits of
hydrocarbon generation theory of kerogen thermal
degeneration.
Ž2. The hydrocarbon-generating potential of kero-
gen is nearly exhausted when vitrinite reflectance
reaches 1.2%. Light oils of high maturity are formed
from condensed pyrobitumen during its higher evolu-
tionary stage. Model of hydrocarbon generation and
evolution of source rocks is presented in this paper.
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