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Machine Learning Assisted Understanding and Discovery of CO2

Reduction Reaction Electrocatalyst
Erhai Hu, Chuntai Liu, Wei Zhang,* and Qingyu Yan*

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ABSTRACT: Electrochemical CO2 reduction reaction (CO2RR)

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is an important process which is a potential way to recycle

excessive CO2 in the atmosphere. Although the electrocatalyst is
the key toward efficient CO2RR, the progress of discovering
effective catalysts is lagging with current methods. Because of the
cost and time efficiency of the modern machine learning (ML)
algorithm, an increasing number of researchers have applied ML to
accelerate the screening of suitable catalysts and to deepen our
understanding in the mechanism. Hence, we reviewed recent
applications of ML in the research of CO2RR by the types of
electrocatalyst. An introduction on the general methodology and a
discussion on the pros and cons for such applications are included.

1. INTRODUCTION In this paper, we intend to summarize recent progresses of

It has become a consensus to reduce carbon dioxide (CO2)
levels in the atmosphere, the major reason for climate change,
to control global warming within a relatively safe level.1
Electrochemical CO2 reduction reaction (CO2RR), as one of
the carbon recycling methods, is promising in this application
because of its ability to turn CO2 into alternative fuels such as
CO, CH4, hydrocarbons, and alcohols. A suitable electro-
catalyst is essential in terms of lowering the energy barrier,
enhancing the catalytic rate, and facilitating high product
selectivity for this reaction. Extensive efforts have been made in
catalyst development for electrochemical CO2 reduction.2 For
example, transition metals3 and their alloys,4 single atom
catalysts (SAC),5 metal oxides,6 MXene,7 and nanostructured
catalysts8 have been shown to be effective for CO2RR.
However, due to the large search space of catalysts, limited
progress has been made compared to the time invested. In
recent years, the development of ab initio methods like density
functional theory (DFT) has helped researchers screen new
catalysts at a faster speed, and it is able to filter out most of the
nonpromising options without further experimentation.
Furthermore, theoretical computation can help us understand
the mechanism better by computing energies for intermediate
and pathways. However, current method still requires a
considerably large amount of time and computational power
to maintain a satisfiable performance.9 Recently, Machine
Learning (ML) emerges as a promising method to accelerate
this process. Given a sufficiently large training data set, a well-
trained ML model could predict the properties (e.g., energy) of
a system with relatively high accuracy at a much faster speed.10
applying ML in the research of CO2RR electrocatalysis. We
will first introduce generic methodologies of ML-assisted
catalyst discovery, followed by current progress in the
understanding and discovery of different types of catalysts.
Finally, we will discuss the challenges presented and possible
future endeavors in this area.
2. GENERAL METHODOLOGY
In general, ML can be either supervised or unsupervised. The
former assumes the availability of a labeled data set and aims to
train an ML model to approximate the mapping from input
features to output, the labels. The latter does not require
labeled data and is designed to learn the patterns without
ground truth. So far, the popular way of ML-based electro-
catalyst screening is the former and labeled data set plays a key
role. Specifically, the supervised ML process starts with training
a model with a data set with a number of data samples, where
each sample consists of an input feature vector and the label of
the corresponding output. The model, once trained, can take in
an input, and produces the modeled, or estimated output.
Naturally, the accuracy of this model can be measured based
on the gap between the derived output and actual/observed
Received: November 28, 2022
Revised: December 13, 2022
Published: January 8, 2023

© 2023 American Chemical Society https://doi.org/10.1021/acs.jpcc.2c08343

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Figure 1. Key elements with examples of ML application in CO2RR (top) and general process of ML during application (bottom).
Figure 2. Schematic of input features matrix and feature selection according to feature importance ranking.
target value.11 In the following subsections, we will introduce
the key elements in ML (Figure 1), specifically in the
application of CO2RR.
2.1. Feature Engineering. As the first step of an ML
process, the input features will be fed into an ML model. They
will be usually in vector or matrix forms for a certain sample
and a whole data set respectively (Figure 2). Features selected
need to well represent the characteristics of the input to enable
efficient training. Typical features describing an electrocatalyst
include geometric features (e.g., atomic radii of compositional
elements and coordination numbers) and electronic features
(e.g., electronegativity, polarizability, valence electron num-
ber). Feature selection is commonly performed before training
the actual model to eliminate redundant features. This may
prevent overfitting and increase accuracy by reducing noise.
Many a feature selection algorithm has been implemented by
measuring the feature importance or statistic correlations
between features.12
2.2. ML Algorithm. An ML algorithm is the core of a
model, which decides the way to process data and learn
features. A few popular ML algorithms have been applied in
this field, such as random forest regression (RFR), support
vector regression (SVR), and gradient boosting regression
(GBR).13−15 Neural networks (NN) give another common
type of ML algorithm which has more flexibility with
information exchange between neurons. Multiple studies
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applied simple NN to predict the adsorption energy of
intermediates such as CO.16−18
As the amount of data in this area continued to grow, deeper
and more complex NN, such as Graph Neural Networks
(GNN), is receiving increasing attentions. In contrast to
traditional ML where input parameters are relatively
independent to each other without capturing much structure
and relational information, GNN realizes the exploration and
utilization of atomic structures of the catalysts. The atoms and
the bonds in such structure can be represented a graph with
nodes and edges.20 For instance, Back et al. use a Crystal
Graph Convolutional Neural Network (CGCNN) to predict
adsorption energy of CO and H based on the initial structure
and connectivity distance of adsorbate and catalyst (Figure 3).
This model achieved a mean absolute error (MAE) of 0.15 eV
respect to the DFT-calculated energy for CO and H
adsorption energy prediction.19 This is considerably accurate
compare to other methods (Table 1). By taking atomic
interactions into consideration, the modeling power of GNN
based models substantially increased, but the required amount
of data is also much more. On the contrary, simpler ML
algorithms may perform better given a small data set.
2.3. Target Properties. As the last step of the process, the
trained model will output a predicted value as the target. The
target property needs to be decided at the very beginning. For
most cases, adsorption or binding energy of certain
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Figure 3. Schematic illustration of CGCNN architecture with atomic
structure input, convolutional layers, fully connected layers, and
binding energy output.19 Reprinted with permission from ref 19.
Copyright 2019 American Chemical Society.
intermediates in CO2RR will be the target because of its direct
relationship to catalytic activity. With this relationship, Tang et
al. quantitatively analyzed the reaction thermodynamics of
different pathways in CO2RR to construct a selectivity map
using only CO and OH binding energy to the catalyst (Figure
4).21 Their derived rules conform well with experiment results
from literature. A ground truth target value will be used during
training with the corresponding input features. This target
value can normally be generated by either DFT computation
or High-Throughput (HT) experimentation.
2.4. Existing Data Sets. There are some existing data sets
and databases storing the features and computed/tested
ground truth value for ML training. Two well-known and
relatively comprehensive material data sets are Materials
Project 2 3 and Open Quantum Materials Database
(OQMD).24 A few other databases specialized in electro-
catalysis have also been established recently. One of them is
the Catalysis-Hub database, with reaction and activation
energies for more than 100 K chemical reactions on catalytic
surfaces collected from near a hundred publications. The data
set offers useful features including displaying atomic structure
and detailed computation settings, data analysis with
interactive plots, and real-time energy prediction with a built-
in ML model.25 Similarly, another database named Open
Catalyst Project (OCP) computed 260 million adsorption
energy exhaustively from a set of adsorbate−catalyst slabs. The
slabs are generated with randomly chosen adsorbates and type
of bulk material, as well as surface and position where the
adsorption happened. This data set is customized for training
and producing ML models, which can be used to screen new
electrocatalytic materials.26
3. RECENT APPLICATIONS OF ML ON CO2RR
ELECTROCATALYST
Different types of catalyst have been used for CO2RR, and the
most popular ones include transition metals,3 metal alloys with
two or more elements,4 and single metal catalysts.5 Some
Table 1. Example of ML Studies of CO Adsorbate Energy Predictions
data set size ML algorithm
Back et al.19 20771 CGCNN
Chen et al.13 171 extreme GBR
Li et al.17 1032 NN
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recent reviews focused on the methodologies and functions of
ML in such research27,28 yet pay much attention to the
difference between application on different types of catalysts.
In this paper, we fill in the gap by introducing the latest
advances according to the type of catalyst.
3.1. Metal. Pure metal electrodes are among the first to be
used as catalysts in electrochemical CO2RR. Representatively,
Hori et al. reported the result of electrochemical CO2RR on a
batch of metal electrodes (e.g., Cu, Pb, Zn, and Ni) and
classified them into four groups based on their major products
(e.g., HCOO−, CO, H2, and >2e−). Because of the limited
number of metal elements, pure metal catalysts can be
thoroughly screened individually with a moderate cost.
However, understanding of this complex reaction process is
still lacking, such as effect of adsorption sites and interaction
between adsorbates. These effects could be well studied with
ML.
Cu with controlled structure and shape has shown superior
catalytic efficiency toward products beyond CO.29 Chen et al.
use ML to study the active sites on Au nanoparticles (AuNP)
responsible to reduce CO2 to CO efficiently.30 First, over 10K
surface sites are identified on AuNP simulated through
molecular dynamic. A two-layer NN with 39 local geometric
features as input was constructed to predict the adsorption
energy of CO and HOCO (ΔECO and ΔEHOCO), two critical
intermediates, on these sites.31 With comparatively small data
set with about 1000 data samples generated from DFT
calculations, an accurate ML model is derived for predicting
ΔECO and ΔEHOCO. Such model is applied to analyze a much
larger scale 10K sites for AuNP and 3K sites for dealloyed
AuNP (Figure 5a), with the prediction results generated
almost instantly. Based on the common understanding that the
CO2RR activity will increase with lower ΔECO and higher
ΔEHOCO,32 active sites, which mainly consist of stepped or
defect surface, could be accurately identified based on the
prediction results (Figure 5b). The better catalytic perform-
ance demonstrated experimentally on dealloyed AuNP33 has
been attributed to the increasing portion of StepUnder111 and
SurfaceDefect sites comparing to pure Au.
Like most of the research, the aforementioned study only
considers the energy of individual adsorbates. Supplementary
adsorbates have also been demonstrated to influence the
catalysis process, but this effect has not been thoroughly
studied yet. For example, coelectrolysis of CO2 and O2 on
copper is able to boost the production of oxygenates and
hydrocarbons to up to 216 times faster. This was attributed to
the introduction of hydroxyl group on copper, which will lower
the energy barrier of CO2RR.34 Hence, the same group
conducted an ML based investigation, focusing on 17
supplementary adsorbates and 289 adsorbate pairs.35 With
these pairs, the energy of two key steps for C2+ and CH4
production,31 *CO dimerization (ΔGCO dimerization) and hydro-
genation (ΔGCO hydrogenation), are predicted using DFT and ML.
Extreme Gradient Boosting Regressor (XGBR) was used to
predict the energy with 6 pairwise features input, including the
catalyst test accuracy
intermetallic MAE: 0.15 eV
SAC RMSE: 0.1652 eV
bimetallic RMSE: 0.22 eV
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Figure 4. Above the potential axis, selectivity maps of CO2RR under different potentials are shown based on binding energy of CO and OH (GCO*
and GOH*). Below the potential axis, experiment results of Hori22 are shown in the map which are fairly consistent with theoretical predictions.21
Reprinted with permission from ref 21. Copyright 2020 Elsevier B.V.

Figure 5. (a) Predicted ΔECO and ΔEHOCO of all sites identified on dealloyed AuNP. (b) Visualization of a value of atoms in dealloyed AuNP,
where a = ΔECO − 1.4423ΔEHOCO. A larger a value indicates better catalytic activity.30 Reprinted with permission from ref 30. Copyright 2019
American Chemical Society.

difference and the average of the valence electron numbers and
covalent radiuses etc. The difference between predicted energy
and that of pristine Cu (100) was plotted as heatmaps (Figure
6, parts b and c). It shows that adsorbates with more unpaired
valence electrons, such as CH, N, CH2, and NH, are likely to
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promote C2+ production by lowering the ΔGCO dimerization, and
almost all adsorbates will reduce ΔGCO hydrogenation to promote
CH4 production.
During liquid phase synthesis of catalyst, additives are
usually introduced to develop a preferable morphology for
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Figure 6. (a) Example structure of *CO dimerization on Cu (100) with the presence of a supplementary adsorbate pair O/O. Orange, gray, red,
and white spheres represent copper, carbon, oxygen, and hydrogen atoms, respectively. (b) Heatmap of the difference between predicted ΔGCO
dimerization and (c) ΔGCO hydrogenation of different adsorbate pairs against that of pristine Cu(100). Reprinted with permission from ref 35. Copyright
2021 American Chemical Society.
efficient CO2RR,36−38 but understanding toward this process is
still lacking. Hence, Guo et al. conducted a series of ML guided
experiments to study the effect of different additives in Cu
synthesis on the catalytic performance.39 In three rounds of
learning, they go through a wide screening of different types of
additives, adding more data points and input variables, and
studying artificial-designed additives with a combination of
features (Figure 7a). In general, faraday efficiency (FE) and
Figure 7. (a) Scheme of three round of learning. Feature importance
of (b) FE-CO and (c) FE-C2+ prediction in the first round of
learning.39 Reprinted with permission from ref 39. Copyright 2021
American Chemical Society.
current density (j) of CO2RR products are the output of ML
models. It was predicted that Sn is most significant for FE-CO
and aliphatic OH group on the organic additive is most
significant for FE-C2+ (Figure 6, parts b and c). Subsequent
experiments reveal that the high FE for organic additives and
Sn is due to the Cu2O phases induced during synthesis, which
has been reported for its high catalytic activity.40,41
3.2. Alloy. Alloy represents an important group of catalyst
in CO2RR. It is possible to tune the electronic properties
through the interaction between different metal components.42
The huge search space of alloying elements and composition
choices impose great challenges particularly for new alloy
catalyst discovery. ML, proven to be able to search efficiently
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35
in huge search spaces of many real-world applications, is a
promising technology to accelerate this process substantially.
Ulissi et al. predict adsorption energy of CO (ΔECO) on
NiGa bimetallics sites exhaustively using NN, where an NN
model was trained iteratively.43 Adsorption configurations of
high certainty are assumed to be trustful. Those with
significant uncertainty are selected automatically for further
refinement or verification using DFT, which produces ground
truth value of the configurations to enhance the training data
set for another round of ML training (Figure 8a). With much
slower DFT being only used for uncertain configurations
instead of all, this proposed process using ML reduces 90% of
the DFT workload compared to traditional non-ML
approaches. Besides, an interesting finding from this work is
that Ni active sites surrounded by Ga atoms demonstrate the
optimal ΔECO like behavior of stepped sites.
In parallel to the above-described effort, Tran and Ulissi
conducted active learning study to find CO2RR and HER
catalyst with ideal CO and H adsorption energy through an
iterative process of DFT and ML (Figure 8b).10 A unique
feature of this study is that only DFT data were included in the
final data set and ML is only used to guide the surface selection
to be calculated using DFT. Four descriptors describing
geometric and electronic features of elements coordinated the
adsorbate were selected as input, and Tree-based Pipeline
Optimization Tool (TPOT)44 was used to choose the best ML
model. In the end, a data set with 42,785 DFT calculations
(ΔECO and ΔEH) was obtained. Based on these data, Cu−Al
bimetallics was identified as a new catalyst to have optimal
ΔECO and ΔEH, which can be seen in the two-dimensional
volcano plots (Figure 9, parts a and b).
Subsequently, the team managed to design and fabricate the
Cu−Al and test its CO2RR activity.45 The best Cu−Al ratio
was found via ML prediction of ΔECO on Cu−Al bimetallics
with different Al concentrations. Optimal morphology and
electrolysis conditions are also studied in different experiments.
As a result, a dealloyed nanoporous Cu−Al on PTFE catalyst
was successfully developed with 2-fold increment in C2H2
selectivity comparing to pure Cu (Figure 9c).
Besides direct analysis on the DFT-produced data set, this
data set was also used to train ML models, such as the
representative aforementioned CGCNN.19 Recently the
CGCNN model has been improved by using the unrelaxed
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Figure 8. Scheme of iterative ML and DFT optimization process. (a) Prediction of ΔECO on NiGa bimetallics43 Reprinted with permission from ref
43. Copyright 2017 American Chemical Society. (b) Selection of catalyst with optimal ΔECO and ΔEH to be included in DFT calculation.10
Reprinted with permission from ref 10. Copyright 2018 Springer Nature.

Figure 9. Two dimensional plots of (a) activity for CO2RR and (b) selectivity toward CO2RR according to ΔECO and ΔEH. (c) FE of gaseous
products on dealloyed Cu−Al at different current density compared with nanoporous Cu and pure Cu.45 Reprinted with permission from ref 45.
Copyright 2020 Springer Nature.

bulk structure of catalyst as input only.46 During training,
binding site atoms are obtained from relaxed adsorbate-catalyst
slab according to a distance criterion. Those atoms are then
labeled on an unrelaxed bare catalyst slab to be used as input
for training (Figure 10a). During new catalyst screening, all
possible adsorption sites will be identified through the graph
conversion of the initial structure, and these labeled site
structures could be used to predict the adsorption energy
(Figure 10b). Besides this representation, the author also
added an attention module and used an ensemble of five
models trained together to further increase the accuracy and
stability. In the end, the LS-CGCNN-ens model could achieve
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over 20% improvement in MAE of ΔGCO compared to its
benchmark CGCNN.
High entropy alloy (HEA) represents an emerging class of
alloy yet is chemically stable. HEA has unique catalytic
properties by combining different metals. Hence, tuning the
composition and concentration is crucial for an optimized
catalytic activity.47 Pedersen et al. studied two set of HEAs,
CoCuGaNiZn and AgAuCuPdPt, by predicting ΔECO and ΔEH
using ML.48 To simplify the possibilities of surface adsorptions,
surface microstructures with only categorical composition
features (Figure 11a) was constructed as input of a Gaussian
process regression (GPR), one of the traditional ML
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Figure 10. (a) Labeled site representation generated during training and (b) the modeling process during application.46 Reprinted with permission
from ref 46. Copyright 2020 American Chemical Society.
Figure 11. (a) Microstructure representation of on top (left), fcc-
hollow (middle), and hcp-hollow (right) adsorption sites.48 The
white, green, blue, and red spheres represent the adsorbate, adsorbing
site, closest surface neighbors, and closest subsurface neighbors,
respectively. Reprinted with permission from ref 48. Copyright 2020
American Chemical Society. (b) Contour plot for adsorption energies
of CO, CH2O and O.49 Selective region is marked by the red square.
Reprinted with permission from ref 49. Copyright 2022 American
Chemical Society.
algorithms. Selectivity toward CO2RR/CORR compared to
HER are studied by analyzing predicted ΔECO and ΔEH. Pure
Cu was confirmed to be the optimal catalyst and locally
optimal compositions of the HEAs can be found according to
the relation.
Roy et al. also studied the selectivity of CuCoNiZnMg and
CuCoNiZnSn HEAs using GPR and kernel ridge regression
(KRR), another traditional ML algorithm, with a similar
microstructure input. Compared to their predecessor, elec-
tronic and geometrical features such as metallic radius and
dipole polarizability are newly introduced into the input. Those
features are more universal and thus the insights gained from
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the corresponding ML models can also shed lights to similar
applications with enhanced generalizability of the deliverables.
Two rounds of screening were conducted from all adsorbates
considered to the most important adsorbates considered. In
the end, 34 HEAs are identified as highly active catalysts
toward methanol generation by screening high CO and H2CO
adsorption energy and relatively low O adsorption energy
(Figure 11b).49
3.3. Single and Dual Atom Catalysts. Single atom
catalyst (SAC) is an emerging class of catalyst with isolated
metal atoms anchored on various supports.50 It possesses
unique catalytic properties because of the quantum size effect
and high utilization of active sites.51 As it was only developed
recently, extensive studies are necessary to be carried out on
SACs with different metal atoms, support, and coordination
environment, where ML could be involved.
Zhou et al. attempt to discover new SAC with different
transition metal (TM) atoms and different nonmetal
coordinated environments using ML.13 Simple electronic and
geometric features are considered to describe the SACs and
filtered according to the Pearson correlation coefficient. For
example, combinations of electronegativity and covalent radius
of metal atoms and coordinated atoms are included in the final
14 features. Using these features, XGBR selected by TPOT
achieved high modeling fidelity with R2 around 0.9 for ΔGCO
prediction, given only about a hundred training data samples
used. The author also computed ΔGH and compared it with
ΔGCO, to find the best catalyst with high CO2RR activity and
low HER activity. As a result, 94 SACs out of 1000 candidates
with potentially high CO2RR efficiency were proposed (Figure
12b).
Dual-atom catalyst (DAC) is an extension of SACs and have
more freedom to adjust the electronic structure of the
adsorption site.52 Wan et al. studied dual-metal-sites catalysts
(DMSCs), which has one TM atom attached to the other one
(Figure 12c), using an analogous method to the previously
mentioned work. GPR is shown to be effective without obvious
reliance on a large-scale data set, which comes at a huge cost of
resource and time. Twenty features describing two TM atoms
and their interaction with the coordinated ring are included.
Unlike many other studies, limiting potential (UL) was selected
as the descriptor for CO2RR, where a smaller absolute value of
UL indicates a lower energy barrier for CO2RR, thus better
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Figure 12. (a) Example of an SAC structure.14 (b) Prediction heat map of ΔGCO on various SACs.13 Blue squares indicate optimal ΔGCO for
CO2RR. (c) Example of a DMSC structure. d) Prediction heat map of limiting potential of various DMSCs. In parts a and c, white, gray, blue,
orange, and green spheres represent H, C, N, TM 1, and TM 2 atoms, respectively. Parts a and c are reprinted with permission from ref 14.
Copyright 2021 American Chemical Society. Parts b and d are reprinted with permission from ref 13. Copyright 2020 American Chemical Society.

Figure 13. (a) Representative RMSE of train set, test set, and test set with CGL. Distribution of ΔECO for SAAs with (b) p-block and (c) d-block
alloying atoms. Ideal range of ΔECO for CO2RR is indicated by dashed lines.15 Reprinted with permission from ref 15. Copyright 2022 Creative
Commons https://creativecommons.org/licenses/by-nc-nd/4.0/legalcode.

CO2RR activity. According to the heat map (Figure 11d),
DMSCs located at the top left possess a higher absolute value
of UL, which may be attributed to the similar electronegativities
of two TM atoms. In contrast, DMSCs with Ag−Mo and Ag−
Co as TM atoms with the lowest absolute value of UL were
considered as high-performance catalysts.
Single atom alloy (SAA) is another type of SAC with
alloying metal atoms dispersed across the host metal surface.53
Wang et al. used DFT to study Cu-based SAA catalysts and
developed an ML model for accurate prediction of ΔECO.15 A
total of 2669 SAA configurations with different Cu facets,
alloying elements, and adsorption sites were identified and
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relaxed using HT DFT. The data were then split into source
and target data sets to train a GBR ML model. Initially,
alloying elements in target data are not included in source data
to test the model’s generalizability. Considering the high
testing error, the model was further trained by adding 10 data
samples from target data set to source data set, which is
referred as cross group learning (CGL). Such CGL turns to be
helpful for boosting the performance and managed to improve
the performance of target data by over 50% (Figure 13a)
without requiring much information on target data.
The author then analyzed ΔECO computed for each SAA
configuration with DFT data. For example, SAA with d-block
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alloying elements shows a wider distribution of ΔECO (Figure
13c), which implies a greater tunability for different catalytic
reactions. Optimal configurations were selected according to
the ideal ΔECO range (Figure 13, parts b and c) and were
further filtered by their ΔEH to find promising SAA catalysts.
4. OUTLOOK
In this Perspective, we introduced the general methodology of
applying ML in CO2RR research. Regardless of the application,
one needs to prepare a sufficiently large data set, select
informative features, train a suitable ML model, and predict a
certain target property. Then, recent research using ML in the
understanding and discovery of pure metal, intermetallic, and
SAC catalyst was demonstrated and discussed.
Though opportunities and advantages brought by ML are
obvious and the research domain looks promising, drawbacks
and challenges of this method still exist inevitably. Powerful
ML algorithms often demand significant training data. For
example, complex models like GNN will outperform traditional
ML models only based on the availability of large-scale data
sets. Generating data samples for ML can be costly, e.g., HT
experiments and DFT with significant overhead for time,
computation, and so on. In this regards, establishment of a
collaborative database, like Catalysis-Hub,25 could solve this
problem to some extent. Further effort is necessary, e.g.,
rigorously and systematically discussing the standardization of
descriptors and methods. In the case of training ML to
approximate DFT, i.e., using DFT to generate training data set,
gaps are there between DFT-derived results and the results
from a real-world implementation. Even ML can accurately
approximate DFT with nearly neglectable error, and the ML
prediction results may not align with real-world experimental
results very well. Hence, the combination of ML and DFT is
more appropriate to guide preliminary screening, while more
formal and practical verification, discovery, and analysis require
HT or manual experiment.
Besides the inherent challenges of computational studies,
there are some other inadequacies, but they can be resolved
through future endeavors:
(a) As discussed, most of the studies focused on adsorption
energy of CO and H. This could only determine the
activity of CO2RR, but the selectivity or dominating
reaction pathways are not distinguishable. Researchers
shall also focus on individual products or pathways and
intermediates beyond CO.
b) More types of catalysts need to be considered with ML-
based approaches. Currently, catalysts studied using ML
are mostly intermetallic and some SACs. Other effective
CO2RR catalysts like metal oxides,6 MXene,7 and
nanostructured catalysts8 shall be studied using ML as
well.
(c) Researchers need to standardize the evaluation of ML
performance with common evaluation metrics and
benchmarking data set. This can enable the research
community to gain qualitative comparison and under-
standing of different proposed approaches and accord-
ingly streamline the optimization process.
(d) Practicality for the synthesis of the discovered catalysts
need to be examined, either before the prediction or in
the post analysis. For example, synthesis of alloys with
certain compositions and some types of SACs may be
impossible or very difficult.
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(e) Some commonly used ML models for CO2RR are black-
box in nature.54 Interpretable ML can be helpful to
understand the model mechanisms and build up trust
and confidence for practical deployment.
Last but not least, ML is more of a supporting technology to
assist users. Domain expertise is a must for research
understanding and results analysis, and naturally a prerequisite
of making full use of this powerful technology for CO2RR
electrocatalyst.
■ AUTHOR INFORMATION
Corresponding Authors
Wei Zhang − Infocomm Technology Cluster, Singapore
Institute of Technology (SIT), Singapore 567739, Singapore;
Email: wei.zhang@singaporetech.edu.sg
Qingyu Yan − Energy Research Institute @ NTU, Singapore
637141, Singapore; School of Material Science and
Engineering, Nanyang Technological University, Singapore
639798, Singapore; Institute of Materials Research and
Engineering, A*STAR, Singapore 138634, Singapore;
orcid.org/0000-0003-0317-3225; Email: alexyan@
ntu.edu.sg
Authors
Erhai Hu − Energy Research Institute @ NTU, Singapore
637141, Singapore; School of Material Science and
Engineering, Nanyang Technological University, Singapore
639798, Singapore; orcid.org/0000-0003-4545-1828
Chuntai Liu − Key Laboratory of Materials Processing and
Mold, Ministry of Education, Zhengzhou University,
Zhengzhou 450002, China; orcid.org/0000-0001-9751-
6270
Complete contact information is available at:
https://pubs.acs.org/10.1021/acs.jpcc.2c08343
Notes
The authors declare no competing financial interest.
Biographies
Erhai Hu completed his Bachelor of Engineering degree in Materials
Engineering at Nanyang Technological University, Singapore. He is
now a Ph.D. student in the Energy Research Institute @ NTU (ERI@
N). His research interests include electrocatalysis, energy storage
materials, and machine learning.
https://doi.org/10.1021/acs.jpcc.2c08343
J. Phys. Chem. C 2023, 127, 882−893
The Journal of Physical Chemistry C
Chuntai Liu is currently a Professor in the School of Material Science
and Engineering at Zhengzhou University. He also serves as deputy
director of the Key Laboratory of Materials Processing and Mold of
the Ministry of Education. His research areas include nanocomposites,
polymer processing, and intelligent materials.
Wei Zhang is currently an Assistant Professor with the Information
and Communications Technology Cluster, Singapore Institute of
Technology (SIT). Dr Zhang serves as an Associate Editor for the
IEEE Internet of Things Journal (IoT-J) as well as the Area Chair,
Track Chair, Review Committee Member, and TPC member of top
conferences such as IJCAI, GLOBECOM, and ICME. His research
interests lie in utilizing artificial intelligence (AI) for smart cities,
especially energy related applications, toward improved user
experience and enhanced sustainability.
Qingyu Yan is currently a Professor in the School of Materials
Science and Engineering at Nanyang Technology University. He
joined the School of Materials Science and Engineering of Nanyang
Technological University as an assistant professor in 2008 and
became a professor in 2018. He is currently the Chair of the
891
pubs.acs.org/JPCC Perspective
Electrochemical Society, Singapore Section. He is a fellow of the
Royal Society of Chemistry since 2018. He has published >300 papers
(with a total citation of >33000 and an h-index of 98) on the research
areas: battery development and thermoelectric materials and electro-
catalytic processes for energy conversion.
■ ACKNOWLEDGMENTS
Q.Y. acknowledges the funding support from Singapore MOE
AcRF Tier 1 under Grant No. 2020-T1-001-031. The authors
would also like to acknowledge the 111 Project (D18023)
from Zhengzhou University for their support for this work.
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