Available online at www.sciencedirect.
com Current Opinion in
ScienceDirect
Definition of photocatalysis: Current understanding
and perspectives
Jiazhe Wu1, Wenyu Zheng1 and Yubin Chen1,2
Photocatalysis is a prospective way to efficiently convert and
store solar energy, which is beneficial for achieving the Sus-
tainable Development Goals (SDGs) proposed by the United
Nations. However, with almost one century research on this
topic, there are still controversies about the definition of
photocatalysis. Wherein, the difference between photocatalytic
and photosynthetic processes is especially argued. In this brief
review, the timeline for major discovery about photocatalysis is
combed and the current understanding of photocatalysis is
summarized. Through analogy with the electrocatalysis, a
revisiting definition towards photocatalysis is presented. The
term “photochemical potential” is proposed based on regarding
photons as reactants. Accordingly, the so-called “photo-
catalytic” and “photosynthetic” processes are both sponta-
neous reactions in the corresponding physical fields, which
reveals that all light-induced catalytic processes can be
generally defined as photocatalysis.
Addresses
1
International Research Center for Renewable Energy (IRCRE), State
Key Laboratory of Multiphase Flow in Power Engineering, Xi’an Jiao-
tong University, Shaanxi, 710049, PR China
2
Integrated Energy Institute, Sichuan Digital Economy Industry
Development Research Institute, Jinniu District, Chengdu, 610036,
China
Corresponding author: Chen, Yubin (ybchen@mail.xjtu.edu.cn)
Current Opinion in Green and Sustainable Chemistry 2022,
33:100580
This review comes from a themed issue on Sustainable Chemistry
and the UN SDGs
Edited by Zhimin Liu and Klaus Kümmerer
https://doi.org/10.1016/j.cogsc.2021.100580
2452-2236/© 2021 Elsevier B.V. All rights reserved.
Introduction
In 2015, the Sustainable Development Goals (SDGs)
were proposed by the United Nations in order to protect
the planet and prosper the human society [1,2]. Among
the 17 SDGs, expanding the usage of affordable clean
energy and controlling climate change are most likely to
be achieved by utilizing solar energy [3,4]. As a clean
and renewable resource, solar energy can be harnessed
and converted into many energy and environmental
systems. Wherein, photocatalysis is a prospective way to
transform solar energy into the value-added chemicals
and dispose environmental pollutants [5e7]. As early as
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Green and Sustainable Chemistry
1921, Baly et al. used the term “photocatalysis” to
describe a photochemical synthesis process in the living
plant [8]. In 1938, Doodeve and Kitchener discovered
that TiO2 could act as a photosensitizer for bleaching
dyes in the presence of oxygen [9]. In 1972, Fujishima
and Honda found the “semiconductor electrochemical
photolysis” phenomenon [10], and then they general-
ized this research area as semiconductor photocatalysis.
In 1977, Bard et al. discovered heterogeneous photo-
catalytic oxidation of cyanide ion in aqueous solutions at
TiO2 powder [11]. In 1979, Inoue et al. reported the
photoelectrocatalytic reduction of CO2 in the aqueous
solution to generate organic chemicals such as formic
acid and methane by using different semiconductor
catalysts [12]. Thus far, studies on photocatalysis have
been extensively carried out in the past decades for
water splitting [13e15], CO2 reduction [16,17], nitro-
gen fixation [18,19], contaminant degradation [20,21],
and organic synthesis [22,23].
With the rapid development of photocatalysis, there are
still controversies about the definition of photocatalysis.
Wherein, the arguments mainly focus on the rationality
of defining a process including non-spontaneous re-
actions as photocatalysis. In this brief review, the current
understanding about the definition of photocatalysis is
summarized. Whereupon, through analogy with the
electrocatalytic processes, a new cognition for the
spontaneity of the photocatalytic process is proposed.
This cognition is based on the energetical favorableness
of the whole process by analyzing the chemical poten-
tials, rather than only considering the thermodynamic
spontaneity of its chemical reaction.
Current understanding of photocatalysis
and photosynthesis
According to the definition of the International Union of
Pure and Applied Chemistry (IUPAC): “photocatalysis
act as a change in the rate of a chemical reaction or its
initiation under the action of ultraviolet, visible, or
infrared radiation in the presence of a substancedthe
photocatalystdthat absorbs light and is involved in the
chemical transformation of the reaction partners [24].”
Although the light-induced catalytic processes are
commonly denoted as photocatalysis in most researches,
the definition of photocatalysis has always been
controversial [25e27]. One standpoint is that the
description of photocatalysis is fundamentally unrea-
sonable [28], because the term “photocatalysis” implies
light acts as the catalyst in the photochemical reactions,
Current Opinion in Green and Sustainable Chemistry 2022, 33:100580
2 Sustainable Chemistry and the UN SDGs
while it actually describes a catalytic process driven by
light. However, the term before “catalysis” can be
regarded as the environment condition (physical field or
biological field) in which the catalytic process takes
place, otherwise the definitions of electrocatalysis, bio-
catalysis, and mechano-catalysis will also be ambiguous.
Besides, some researchers pointed out that if photo-
catalysis is a catalytic process, the presence of catalyst
should only change the kinetic rate rather than ther-
modynamic limits of the photochemical process. Based
on this perspective, they classified these photochemical
reactions into photocatalytic and photosynthetic pro-
cesses according to the thermodynamic spontaneity of
the chemical reactions [29e31]. As depicted in Figure 1,
a photochemical process with reaction DG > 0 (uphill)
is attributed to photosynthesis, including the overall
water photolysis, CO2 reduction, and the natural
photosynthesis while the process with reaction DG < 0
(downhill) is actually the photocatalysis, such as
hydrogen evolution reaction with sacrificial reagents.
Based on this viewpoint, Osterloh proposed various
types of photocatalytic and photosynthetic devices
respectively for water splitting and specified the
limiting functions and parameters for each one [32].
Further naming photoelectrochemical processes was
suggested by Rajeshwar et al. [33], where photocatalytic
and photosynthetic processes were distinguished by the
free-energy change of the involved chemical reactions.
However, it is worth noting whether it is rigorous to
define the entire physicochemical processes based on
the thermodynamic of the chemical reactions. In other
word, it is necessary to consider not only the influence of
thermodynamic fields (containing temperature T, pres-
sure P, etc.), but also the effects of other physical fields
on the entire photochemical processes, to reflect the
reaction spontaneity. A similar case is the electro-
catalysis, in which the external electricity is added to
drive chemical reactions. The terms “electrocatalysis”
Figure 1
Illustration of photosynthesis and photocatalysis according to the ther-
modynamic spontaneity of chemical reactions.
Current Opinion in Green and Sustainable Chemistry 2022, 33:100580
and “electrosynthesis” are commonly used in electro-
chemistry. The electrosynthesis refers to a process with
the synthesis of chemical compounds in an electro-
chemical cell [34]. The electrocatalysis means that the
electrochemical reaction proceeds with catalysts
participating in the process [35]. However, the defini-
tions of electrocatalysis and electrosynthesis are not
directly distinguished according to the Gibbs free
energy change of the chemical reactions. Some elec-
trosynthesis reactions are also electrocatalytic reactions
[36]. At the same time, the electro-assisted water
splitting is generally named as electrocatalytic water
splitting [37e39]. If we take the water splitting reaction
(H2 O/H2 þ 1=2O2 ) as an example to identify the
spontaneity of the electrochemical and photochemical
reaction, it seems to be less controversial whether
“electrocatalysis” is a catalytic process. Therefore, we
will take the electrocatalytic water splitting as a begin-
ning to identify the spontaneity of the electro-assisted
chemical reaction.
Analogy analysis of electrocatalytic water
splitting
For electrocatalytic processes, there are many so-called
non-spontaneous (DG > 0) reactions, in which the
electrolysis of water is one typical example.
H2 O / H2 þ 1=2O2 DG0 >0 (1)
According to the definition of photocatalysis and
photosynthesis, this process should be defined as
“electrosynthesis” rather than “electrocatalysis.” To
avoid this argument, electrochemical researchers have
proposed the concept of electrochemical potential (mai )
[40]. For species i with charge zi in a phase, the mai is:
mai ¼ mai þ zi Ffa (2)
In this equation, mai is the chemical potential, F is the
Faraday constant, fa is the electric potential of a phase.
According to this definition, when calculating the elec-
trochemical potential of one species in an electro-
chemical system, both the thermodynamic energy of the
chemical species and the added electric energy should
be considered. Therefore, the electrochemical free
energy (G) instead of the free energy (G) is used as a
criterion to determine whether a reaction can proceed
spontaneously, and its relationship with the electro-
chemical potential is:
 
vG
mai ¼ (3)
vni T ;P;njsi
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In this equation, ni is the mole number of species i in a
phase. The subscript T ; P; njsi means that the tem-
perature, pressure, and mole number of other species
keep constant. Obviously, like substances present in
electrochemical systems, the electrons (e , z ¼  1)
also have the chemical potential. For the electrons in a
phase, the mae is [40]:
mae ¼ mae  Ffa
mae describes the average energy of the effective electrons
in a phase. In solid state physics, it has a more familiar
definitiondthe Fermi energy level [40e42].
For the electrolytic water splitting (Figure 2a), the
anode and cathode of the electrolytic cell are two
identical Pt electrodes (PtA anode and PtC cathode), to
ensure that the chemical potentials of electrons at both
electrodes are identical in vacuum. A bias Vapp is applied
between the two electrodes and the electrolyte is
assumed in an acidic environment. At the anode, H2O is
oxidized and electrons are transferred to the PtA:
H2 O / 2Hþ þ 1=2O2 þ 2e ðPtA Þ
At the cathode, Hþ is reduced by the electrons:
2Hþ þ 2e ðPtC Þ/H2
Then the expression of the whole reaction is:
H2 O þ 2e ðPtC Þ / H2 þ 1 = 2O2 þ 2e ðPtA Þ
Figure 2
(a) Scheme of electrocatalytic water splitting process. (b) Gibbs free energy change when the electrochemical potential is considered.
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Definition of photocatalysis Wu et al. 3
When the electrochemical potentials of electrons (mPte
A
and me ) are considered in reaction (7), the DG0 of this
Pt C
reaction could be presented as:



DG0 ¼ mH2 þ 1 = 2mO2  mH2 O  2F fPtA  fPtC (8)
It is noted that, in this equation, the
(4) ðmH2 þ1 =2mO2 mH2 O Þ item is DG0 of the reaction (1),
and the ðfPtA fPtC Þ item is equal to Vapp (when
ignoring the external circuit resistance). Therefore, the
DG0 can be rewritten as:
DG0 ¼ DG0  2FVapp (9)
where upon as shown in Figure 2b the electrolytic water
reaction can proceed “spontaneously” when the applied
bias is large enough to make DG0 < 0. In this process, the
electrocatalyst plays the same role as other catalytic sys-
tems, only kinetically accelerating but not thermodynami-
cally influencing the electrocatalytic process. In other
words, the electrocatalyst does not change the reaction
equilibrium.
(5)
Revisiting the definition of photocatalysis
As we know, there are two laws in photochemical pro-
cesses. The first one states that only the light absorbed by
the substance can cause photochemical changes, while
(6) the second one is the famous photoelectric effect equa-
tion [43,44]. Both of them imply that the photon is a piece
of energy putting into the reaction system. However,
some ideas believed that photons can work as reactants in
physicochemical processes [45e47]. Based on this
DG0 comprehension, a revisiting definition of photocatalysis is
(7) proposed by analogy with electrochemical process.
Current Opinion in Green and Sustainable Chemistry 2022, 33:100580
4 Sustainable Chemistry and the UN SDGs
Photocatalytic water splitting in the acidic electrolyte is
used as an example to discuss the suspended photo-
catalytic systems. As described in Figure 3a, the mono-
chromatic photons with a frequency of n excite the
electrons from the valence band to the conduction band.
Then the excited electrons transfer to the surface and
reduce the Hþ . The electrons in H2 O are transferred to
the valence band where the electron energy level is
lower (for better illustration, the concept of holes is not
used here). Thus, the reaction process could be
described as:
hn þ e ðVÞ/e ðCÞ
2Hþ þ 2e ðCÞ/H2
H2 O / 2Hþ þ 1=2O2 þ 2e ðVÞ
where e ðVÞ denotes the electron in valance band and
e ðCÞ denotes the electron in conduction band. Then the
expression of the whole reaction is:
H2 O þ 2hn/H2 þ 1=2O2 DG~0
It is noted that in reaction (13), the photons with the
energy of hn appears as the “reactant”. To distinguish it
from reaction (1), here, we introduce the photochemical
free energy G~0. According to the definition of chemical
potential, for photoexcited species i in a phase, the
photochemical potential m ~ a i could be expressed as
follow:
 ~
vG
~ai ¼
m ~ n ap
¼ mai þ m (14)
vni T ;P;jsi
Figure 3
(a) Scheme of photocatalytic water splitting. (b) Gibbs free energy change when considering photons as the reactant of photocatalytic water splitting.
Current Opinion in Green and Sustainable Chemistry 2022, 33:100580
~ n ap denotes the photochemical potential of absor-
where m
bed photons with frequency n.
It is generally believed that the chemical potential of
photons is 0, so that electromagnetic waves with
different frequencies, directions, and intensities can
exist stably in the same “phase” without mutual con-
version of photon energy [48,49]. Therefore, the word
“absorbed” is added before “photon” to emphasize the
chemical potential of the photons absorbed by photo-
chemical systems. m ~ n ap could be calculated as:
(10) ~ vap ¼ NA hn
m (15)
where NA denotes the Avogadro constant, h denotes the
(11) Planck constant. Then turning back to reaction (13), we
obtain that:
(12)
DG~0 ¼ DG0  2NA hn (16)
Analogous to the concept of electrochemical free
energy, we can conclude that if the m~ n ap is high enough
(13)
~
to make DG0 < 0, the photochemical process could
react spontaneously (Figure 3b). When the reaction
system is under dark condition, the DG~0 is uphill so
that the process cannot take place. After introducing
the light field, the DG~0 is altered into downhill by
adding the photochemical potential of absorbed pho-
tons at the reactant side, and the photocatalytic pro-
cess occurs. Similar to electrocatalytic water splitting,
the photocatalyst does not change the reaction equi-
librium. Therefore, by considering photons as the re-
actants, all light-induced catalytic processes can be
generally defined as photocatalysis, regardless of the
free energy change of chemical reactions.
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Concluding remarks
The controversies about photocatalysis and photosyn-
thesis always focus on the thermodynamic spontaneity of
the chemical reactions involved in the processes.
Whereupon the observation and analysis of a whole pro-
cess is limited. In this brief review, a renewed criterion of
photochemical free energy is proposed by introducing the
photochemical potential of absorbed photons. The so-
called “photocatalytic” and “photosynthetic” processes
are both spontaneous reactions in the corresponding
physical fields. The classification method according to
thermodynamic spontaneity of chemical reactions could
be rectified under the new cognition. In this vision, the
photocatalysts in photochemical systems act as the
“mediator” between the reactants and photons (a special
reactant) to accelerate the kinetics process, which is
exactly what the catalysts does.
Notes
The authors declare no competing financial interest.
Declaration of competing interest
The authors declare that they have no known competing
financial interests or personal relationships that could
have appeared to influence the work reported in this
article.
Acknowledgements
Y.C. would like to thank the financial support from the
National Natural Science Foundation of China (Nos.
51888103 and 52076177), Shaanxi Technical Innovation
Guidance Project (No. 2018HJCG-14), and Sichuan
Science and Technology Program (No. 2021YFSY0047).
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