High throughput screening of single atomic catalysts with optimized local structures for the electrochemical oxygen reduction by machine learning

Single atomic catalysts(SACs),especially metal-nitrogen doped carbon(M-NC)catalysts,have been extensively explored for the electrochemical oxygen reduction reaction(ORR),owing to their high activity and atomic utilization efficiency.However,there is still a lack of systematic screening and optimization of local structures surrounding active centers of SACs for ORR as the local coordination has an essential impact on their electronic structures and catalytic performance.Herein,we systematic study the ORR catalytic performance of M-NC SACs with different central metals and environmental atoms in the first and second coordination sphere by using density functional theory(DFT)calculation and machine learning(ML).The geometric and electronic informed overpotential model(GEIOM)based on random forest algorithm showed the highest accuracy,and its R^(2) and root mean square errors(RMSE)were 0.96 and 0.21,respectively.30 potential high-performance catalysts were screened out by GEIOM,and the RMSE of the predicted result was only 0.12 V.This work not only helps us fast screen high-performance catalysts,but also provides a low-cost way to improve the accuracy of ML models.

Electrochemical Kinetic Modulators in Lithium–Sulfur Batteries:From Defect-Rich Catalysts to Single Atomic Catalysts

Lithium–sulfur batteries exhibit unparalleled merits in theoretical energy density(2600 W h kg^(-1))among next-generation storage systems.However,the sluggish electrochemical kinetics of sulfur reduction reactions,sulfide oxidation reactions in the sulfur cathode,and the lithium dendrite growth resulted from uncontrollable lithium behaviors in lithium anode have inhibited high-rate conversions and uniform deposition to achieve high performances.Thanks to the“adsorption-catalysis”synergetic effects,the reaction kinetics of sulfur reduction reactions/sulfide oxidation reactions composed of the delithiation of Li_(2)S and the interconversions of sulfur species are propelled by lowering the delithiation/diffusion energy barriers,inhibiting polysulfide shuttling.Meanwhile,the anodic plating kinetic behaviors modulated by the catalysts tend to uniformize without dendrite growth.In this review,the various active catalysts in modulating lithium behaviors are summarized,especially for the defect-rich catalysts and single atomic catalysts.The working mechanisms of these highly active catalysts revealed from theoretical simulation to in situ/operando characterizations are also highlighted.Furthermore,the opportunities of future higher performance enhancement to realize practical applications of lithium–sulfur batteries are prospected,shedding light on the future practical development.

Optimizing high-coordination shell of Co-based single-atom catalysts for efficient ORR and zinc-air batteries

Atom-level modulation of the coordination environment for single-atom catalysts(SACs)is considered as an effective strategy for elevating the catalytic performance.For the MNxsite,breaking the symmetrical geometry and charge distribution by introducing relatively weak electronegative atoms into the first/second shell is an efficient way,but it remains challenging for elucidating the underlying mechanism of interaction.Herein,a practical strategy was reported to rationally design single cobalt atoms coordinated with both phosphorus and nitrogen atoms in a hierarchically porous carbon derived from metal-organic frameworks.X-ray absorption spectrum reveals that atomically dispersed Co sites are coordinated with four N atoms in the first shell and varying numbers of P atoms in the second shell(denoted as Co-N/P-C).The prepared catalyst exhibits excellent oxygen reduction reaction(ORR)activity as well as zinc-air battery performance.The introduction of P atoms in the Co-SACs weakens the interaction between Co and N,significantly promoting the adsorption process of ^(*)OOH,resulting in the acceleration of reaction kinetics and reduction of thermodynamic barrier,responsible for the increased intrinsic activity.Our discovery provides insights into an ultimate design of single-atom catalysts with adjustable electrocatalytic activities for efficient electrochemical energy conversion.

Structure design and electrochemical properties of carbon-based single atom catalysts in energy catalysis:A review

Single atom catalysts(SACs) possessing regulated electronic structure, high atom utilization, and superior catalytic efficiency have been studied in almost all fields in recent years. Carbon-based supporting SACs are becoming popular materials because of their low cost, high electron conductivity, and controllable surface property. At the stage of catalysts preparation, the rational design of active sites is necessary for the substantial improvement of activity of catalysts. To date, the reported design strategies are mainly about synthesis mechanism and synthetic method. The level of understanding of design strategies of carbon-based single atom catalysts is requiring deep to be paved. The design strategies about manufacturing defects and coordination modulation of catalysts are presented. The design strategies are easy to carry out in the process of drawing up preparation routes. The components of carbon-based SACs can be divided into two parts: active site and carbon skeleton. In this review, the manufacture of defects and coordination modulation of two parts are introduced, respectively. The structure features and design strategies from the active sites and carbon skeletons to the overall catalysts are deeply discussed.Then, the structural design of different nano-carbon SACs is introduced systematically. The characterization of active site and carbon skeleton and the detailed mechanism of reaction process are summarized and analyzed. Next, the applications in the field of electrocatalysis for oxygen conversion and hydrogen conversion are illustrated. The relationships between the superior performance and the structure of active sites or carbon skeletons are discussed. Finally, the conclusion of this review and prospects on the abundant space for further promotion in broader fields are depicted. This review highlights the design and preparation thoughts from the parts to the whole. The detailed and systematic discussion will provide useful guidance for design of SACs for readers.

Precise construction of RuPt dual single-atomic sites to optimize oxygen electrocatalytic behaviors for high-performance Zn-air batteries

The development of redox bifunctional electrocatalysts with high performance,low cost,and long lifetimes is essential for achieving clean energy goals.This study proposed an atom capture strategy for anchoring dual single atoms(DSAs)in a zinc-zeolitic imidazolate framework(Zn-ZIF),followed by calcination under an N_(2) atmosphere to synthesize ruthenium-platinum DSAs supported on a nitrogendoped carbon substrate(RuPt DSAs-NC).Theoretical calculations showed that the degree of Ru 5dxz-~*O 2p_x orbital hybridization was high when^(*)O was adsorbed at the Ru site,indicating enhanced covalent hybridization of metal sites and oxygen ligands,which benefited the adsorption of intermediate species.The presence of the RuPtN_6 active center optimized the absorption-desorption behavior of intermediates,improving the electrocatalytic performance of the oxygen reduction reaction(ORR)and the oxygen evolution reaction(DER),RuPt DSAs-NC exhibited a 0.87 V high half-wave potential and a 268 mV low overpotential at 10 mA cm^(-2)in an alkaline environment.Furthermore,rechargeable zinc-air batteries(ZABs)achieved a peak power density of 171 MW cm^(-2).The RuPt DSAs-NC demonstrated long-term cycling for up to 500 h with superior round-trip efficiency.This study provided an effective structural design strategy to construct DSAs active sites for enhanced electrocata lytic performance.

Single-atom catalysts based on polarization switching of ferroelectric In_(2)Se_(3) for N_(2) reduction

The polarization switching plays a crucial role in controlling the final products in the catalytic pro-cess.The effect of polarization orientation on nitrogen reduction was investigated by anchoring transition metal atoms to form active centers on ferroelectric material In_(2)Se_(3).During the polariza-tion switching process,the difference in surface electrostatic potential leads to a redistribution of electronic states.This affects the interaction strength between the adsorbed small molecules and the catalyst substrate,thereby altering the reaction barrier.In addition,the surface states must be considered to prevent the adsorption of other small molecules(such as *O,*OH,and *H).Further-more,the V@↓-In_(2)Se_(3) possesses excellent catalytic properties,high electrochemical and thermody-namic stability,which facilitates the catalytic process.Machine learning also helps us further ex-plore the underlying mechanisms.The systematic investigation provides novel insights into the design and application of two-dimensional switchable ferroelectric catalysts for various chemical processes.

Preparation of single atom catalysts for high sensitive gas sensing

Single atom catalysts(SACs)have garnered significant attention in the field of catalysis over the past decade due to their exceptional atom utilization efficiency and distinct physical and chemical properties.For the semiconductor-based electrical gas sensor,the core is the catalysis process of target gas molecules on the sensitive materials.In this context,the SACs offer great potential for highly sensitive and selective gas sensing,however,only some of the bubbles come to the surface.To facilitate practical applications,we present a comprehensive review of the preparation strategies for SACs,with a focus on overcoming the challenges of aggregation and low loading.Extensive research efforts have been devoted to investigating the gas sensing mechanism,exploring sensitive materials,optimizing device structures,and refining signal post-processing techniques.Finally,the challenges and future perspectives on the SACs based gas sensing are presented.

Progresses and Prospects of Asymmetrically Coordinated Single Atom Catalysts for Lithium-Sulfur Batteries

Lithium-sulfur batteries(LSBs)are widely regarded as promising next-generation batteries due to their high theoretical specific capacity and low material cost.However,the practical applications of LSBs are limited by the shuttle effect of lithium polysulfides(LiPSs),electronic insulation of charge and discharge products,and slow LiPSs conversion reaction kinetics.Accordingly,the introduction of catalysts into LSBs is one of the effective strategy to solve the issues of the sluggished LiPS conversion.Because of their nearly 100%atom utilization and high electrocatalytic activity,single-atom catalysts(SACs)have been widely used as reaction mediators for LSBs’reactions.Excitingly,the SACs with asymmetric coordination structures have exhibited intriguing electronic structures and superior catalytic activities when compared to the traditional M-N_(4)active sites.In this review,we systematically describe the recent advancements in the installation of asymmetrically coordinated single-atom structure as reactions catalysts in LSBs,including asymmetrically nitrogen coordinated SACs,heteroatom coordinated SACs,support effective asymmetrically coordinated SACs,and bimetallic coordinated SACs.Particularly noteworthy is the discussion of the catalytic conversion mechanism of LiPSs spanning asymmetrically coordinated SACs.Finally,a perspective on the future developments of asymmetrically coordinated SACs in LSB applications is provided.

Aqueous Zinc Batteries with Ultra‑Fast Redox Kinetics and High Iodine Utilization Enabled by Iron Single Atom Catalysts

Rechargeable aqueous zinc iodine(ZnǀǀI_(2))batteries have been promising energy storage technologies due to low-cost position and constitutional safety of zinc anode,iodine cathode and aqueous electrolytes.Whereas,on one hand,the low-fraction utilization of electrochemically inert host causes severe shuttle of soluble polyiodides,deficient iodine utilization and sluggish reaction kinetics.On the other hand,the usage of high mass polar electrocatalysts occupies mass and volume of electrode materials and sacrifices device-level energy density.Here,we propose a“confinement-catalysis”host composed of Fe single atom catalyst embedding inside ordered mesoporous carbon host,which can effectively confine and catalytically convert I_(2)/I^(−)couple and polyiodide intermediates.Consequently,the cathode enables the high capacity of 188.2 mAh g^(−1)at 0.3 A g^(−1),excellent rate capability with a capacity of 139.6 mAh g^(−1)delivered at high current density of 15 A g^(−1)and ultra-long cyclic stability over 50,000 cycles with 80.5%initial capacity retained under high iodine loading of 76.72 wt%.Furthermore,the electrocatalytic host can also accelerate the I^(+)↔I_(2)conversion.The greatly improved electrochemical performance originates from the modulation of physicochemical confinement and the decrease of energy barrier for reversible I−/I_(2)and I_(2)/I^(+)couples,and polyiodide intermediates conversions.

The role of copper in enhancing the performance of heteronuclear diatomic catalysts for the electrochemical CO_(2)conversion to C_(1) chemicals

Diatomic catalysts(DACs)with two adjacent metal atoms supported on graphene can offer diverse functionalities,overcoming the inherent limitations of single atom catalysts(SACs).In this study,density functional theory calculations were conducted to investigate the reactivity of the carbon dioxide(CO_(2))reduction reaction(CO_(2)RR)on metal sites of both DACs and SACs,as well as their synergistic effects on activity and selectivity.Calculation of the Gibbs free energies of CO_(2)RR and associated values of the limiting potentials to generate C_(1) products showed that Cu acts as a promoter rather than an active catalytic centre in the catalytic CO_(2)conversion on heteronuclear DACs(CuN_(4)-MN_(4)),improving the catalytic activity on the other metal compared to the related SAC MN_(4).Cu enhances the initial reduction of CO_(2)by promoting orbital hybridization between the key intermediate*COOH 2p-orbitals and the metals 3d-orbitals around the Fermi level.This degree of hybridization in the DACs CuN_(4)-MN_(4) decreases from Fe to Co,Ni,and Zn.Our work demonstrates how Cu regulates the CO_(2)RR performance of heteronuclear DACs,offering an effective approach to designing practical,stable,and high-performing diatomic catalysts for CO_(2)electroreduction.

Recent advances in regulating the performance of acid oxygen reduction reaction on carbon-supported non-precious metal single atom catalysts

Developing high performance and low-cost catalysts for oxygen reduction reaction(ORR)in challenging acid condition is vital for proton-exchange-membrane fuel cells(PEMFCs).Carbon-supported nonprecious metal single atom catalysts(SACs)have been identified as potential catalysts in the field.Great advance has been obtained in constructing diverse active sites of SACs for improving the performance and understanding the fundamental principles of regulating acid ORR performance.However,the ORR performance of SACs is still unsatisfactory.Importantly,microenvironment adjustment of SACs offers chance to promote the performance of acid ORR.In this review,acid ORR mechanism,attenuation mechanism and performance improvement strategies of SACs are presented.The strategies for promoting ORR activity of SACs include the adjustment of center metal and its microenvironment.The relationship of ORR performance and structure is discussed with the help of advanced experimental investigations and theoretical calculations,which will offer helpful direction for designing advanced SACs for ORR.

Single-atom Pt on carbon nanotubes for selective electrocatalysis

Utilizing supported single atoms as catalysts presents an opportunity to reduce the usage of critical raw materials such as platinum,which are essential for electrochemical reactions such as hydrogen oxidation reaction(HOR).Herein,we describe the synthesis of a Pt single electrocatalyst inside single-walled carbon nanotubes(SWCNTs)via a redox reaction.Characterizations via electron microscopy,X-ray photoelectron microscopy,and X-ray absorption spectroscopy show the single-atom nature of the Pt.The electrochemical behavior of the sample to hydrogen and oxygen was investigated using the advanced floating electrode technique,which minimizes mass transport limitations and gives a thorough insight into the activity of the electrocatalyst.The single-atom samples showed higher HOR activity than state-of-the-art 30%Pt/C while almost no oxygen reduction reaction activity in the proton exchange membrane fuel cell operating range.The selective activity toward HOR arose as the main fingerprint of the catalyst confinement in the SWCNTs.

Atomically dispersed Fe sites on hierarchically porous carbon nanoplates for oxygen reduction reaction

Developing cost-effective,robust and stable non-precious metal catalysts for oxygen reduction reaction(ORR) is of paramount importance for electrochemical energy conversion devices such as fuel cells and metal-air batteries.Although Fe-N-C single atom catalysts(SACs) have been hailed as the most promising candidate due to the optimal binding strength of ORR intermediates on the Fe-N_(4) sites,they suffer from serious mass transport limitations as microporous templates/substrates,i.e.,zeolitic imidazolate frameworks(ZIFs),are usually employed to host the active sites.Motivated by this challenge,we herein develop a hydrogen-bonded organic framework(HOF)-assisted pyrolysis strategy to construct hierarchical micro/mesoporous carbon nanoplates for the deposition of atomically dispersed Fe-N_(4) sites.Such a design is accomplished by employing HOF nanoplates assembled from 2-aminoterephthalic acid(NH_(2)-BDC) and p-phenylenediamine(PDA) as both soft templates and C,N precursors.Benefitting from the structural merits inherited from HOF templates,the optimized catalyst(denoted as Fe-N-C SAC-950) displays outstanding ORR activity with a high half-wave potential of 0.895 V(vs.reversible hydrogen electrode(RHE)) and a small overpotential of 356 mV at 10 mA cm^(-2) for the oxygen evolution reaction(OER).More excitingly,its application potential is further verified by delivering superb rechargeability and cycling stability with a nearly unfading charge-discharge gap of 0.72 V after 160 h.Molecular dynamics(MD) simulations reveal that micro/mesoporous structure is conducive to the rapid mass transfer of O_(2),thus enhancing the ORR performance.In situ Raman results further indicate that the conversion of O_(2) to~*O_(2)-the rate-determining step(RDS) for Fe-N-C SAC-950.This work will provide a versatile strategy to construct single atom catalysts with desirable catalytic properties.

Cooperation between single atom catalyst and support to promote nitrogen electroreduction to ammonia:A theoretical insight

The co-catalysis between single atom catalyst(SAC)and its support has recently emerged as a promising strategy to synergistically boost the catalytic activity of some complex electrochemical reactions,encompassing multiple intermediates and pathways.Herein,we utilized defective BC_(3)monolayer-supported SACs as a prototype to investigate the cooperative effects of SACs and their support on the catalytic performance of the nitrogen reduction reaction(NRR)for ammonia(NH_(3))production.The results showed that these SACs can be firmly stabilized on these defective BC_(3)supports with high stability against aggregation.Furthermore,co-activation of the inert N_(2)reactant was observed in certain embedded SACs and their neighboring B atoms on certain BC3 sheets due to the noticeable charge transfer and significant N–N bond elongation.Our high-throughput screening revealed that the Mo/DV_(CC)and W/DV_(CC)exhibit superior NRR catalytic performance,characterized by a low limiting potential of−0.33 and−0.43 V,respectively,which can be further increased under acid conditions based on the constant potential method.Moreover,varying NRR catalytic activities can be attributed to the differences in the valence state of active sites.Remarkably,further microkinetic modeling analysis displayed that the turnover frequency of N_(2)–to–NH_(3)conversion on Mo/DV_(CC)is as large as 1.20×10^(−3)s^(−1)site^(−1) at 700 K and 100 bar,thus guaranteeing its ultra-fast reaction rate.Our results not only suggest promising advanced electrocatalysts for NRR but also offer an effective avenue to regulate the electrocatalytic performance via the co-catalytic metal–support interactions.

Crystallographically vacancy‐induced MOF nanosheet as rational single‐atom support for accelerating CO_(2) electroreduction to CO

To attain a circular carbon economy and resolve CO_(2) electroreduction technology obstacles,single‐atom catalysts(SACs)have emerged as a logical option for electrocatalysis because of their extraordinary catalytic activity.Among SACs,metal–organic frameworks(MOFs)have been recognized as promising support materials because of their exceptional ability to prevent metal aggregation.This study shows that atomically dispersed Ni single atoms on a precisely engineered MOF nanosheet display a high Faradaic efficiency of approximately 100% for CO formation in H‐cell and three‐compartment microfluidic flow‐cell reactors and an excellent turnover frequency of 23,699 h^(−1),validating their intrinsic catalytic potential.These results suggest that crystallographic variations affect the abundant vacancy sites on the MOF nanosheets,which are linked to the evaporation of Zn‐containing organic linkers during pyrolysis.Furthermore,using X‐ray absorption spectroscopy and density functional theory calculations,a comprehensive investigation of the unsaturated atomic coordination environments and the underlying mechanism involving CO^(*) preadsorbed sites as initial states was possible and provided valuable insights.

Metal-N_(4) model single‐atom catalyst with electroneutral quadri‐pyridine macrocyclic ligand for CO_(2) electroreduction

Metal–N–C single‐atom catalysts,mostly prepared from pyrolysis of metalorganic precursors,are widely used in heterogeneous electrocatalysis.Since metal sites with diverse local structures coexist in this type of material and it is challenging to characterize the local structure,a reliable structure–property relationship is difficult to establish.Conjugated macrocyclic complexes adsorbed on carbon support are well‐defined models to mimic the singleatom catalysts.Metal–N_(4) site with four electroneutral pyridine‐type ligands embedded in a graphene layer is the most commonly proposed structure of the active site of single‐atom catalysts,but its molecular counterpart has not been reported.In this work,we synthesized the conjugated macrocyclic complexes with a metal center(Co,Fe,or Ni)coordinated with four electroneutral pyridinic ligands as model catalysts for CO_(2) electroreduction.For comparison,the complexes with anionic quadri‐pyridine macrocyclic ligand were also prepared.The Co complex with the electroneutral ligand expressed a turnover frequency of CO formation more than an order of magnitude higher than that of the Co complex with the anionic ligand.Constrained ab initio molecular dynamics simulations based on the well‐defined structures of the model catalysts indicate that the Co complex with the electroneutral ligand possesses a stronger ability to mediate electron transfer from carbon to CO_(2).

Accelerating the Screening of Modified MA_(2)Z_(4) Catalysts for Hydrogen Evolution Reaction by Deep Learning-Based Local Geometric Analysis

Machine learning(ML)integrated with density functional theory(DFT)calculations have recently been used to accelerate the design and discovery of single-atom catalysts(SACs)by establishing deep structure–activity relationships.The traditional ML models are always difficult to identify the structural differences among the single-atom systems with different modification methods,leading to the limitation of the potential application range.Aiming to the structural properties of several typical two-dimensional MA_(2)Z_(4)-based single-atom systems(bare MA_(2)Z_(4) and metal single-atom doped/supported MA_(2)Z_(4)),an improved crystal graph convolutional neural network(CGCNN)classification model was employed,instead of the traditional machine learning regression model,to address the challenge of incompatibility in the studied systems.The CGCNN model was optimized using crystal graph representation in which the geometric configuration was divided into active layer,surface layer,and bulk layer(ASB-GCNN).Through ML and DFT calculations,five potential single-atom hydrogen evolution reaction(HER)catalysts were screened from chemical space of 600 MA_(2)Z_(4)-based materials,especially V_(1)/HfSn_(2)N_(4)(S)with high stability and activity(Δ_(GH*)is 0.06 eV).Further projected density of states(pDOS)analysis in combination with the wave function analysis of the SAC-H bond revealed that the SAC-dz^(2)orbital coincided with the H-s orbital around the energy level of−2.50 eV,and orbital analysis confirmed the formation ofσbonds.This study provides an efficient multistep screening design framework of metal single-atom catalyst for HER systems with similar two-dimensional supports but different geometric configurations.

Tailoring local structures of atomically dispersed copper sites for highly selective CO_(2) electroreduction

Atomically‐dispersed copper sites coordinated with nitrogen‐doped carbon(Cu–N–C)can provide novel possibilities to enable highly selective and active electrochemical CO_(2) reduction reactions.However,the construction of optimal local electronic structures for nitrogen‐coordinated Cu sites(Cu–N_(4))on carbon remains challenging.Here,we synthesized the Cu–N–C catalysts with atomically‐dispersed edge‐hosted Cu–N_(4) sites(Cu–N_(4)C_(8))located in a micropore between two graphitic sheets via a facile method to control the concentration of metal precursor.Edge‐hosted Cu–N_(4)C_(8) catalysts outperformed the previously reported M–N–C catalysts for CO_(2)‐to‐CO conversion,achieving a maximum CO Faradaic efficiency(FECO)of 96%,a CO current density of–8.97 mA cm^(–2) at–0.8 V versus reversible hydrogen electrode(RHE),and over FECO of 90%from–0.6 to–1.0 V versus RHE.Computational studies revealed that the micropore of the graphitic layer in edge‐hosted Cu–N_(4)C_(8) sites causes the d‐orbital energy level of the Cu atom to shift upward,which in return decreases the occupancy of antibonding states in the*COOH binding.This research suggests new insights into tailoring the locally coordinated structure of the electrocatalyst at the atomic scale to achieve highly selective electrocatalytic reactions.

Exploring the Roles of Single Atom in Hydrogen Peroxide Photosynthesis

This comprehensive review provides a deep exploration of the unique roles of single atom catalysts(SACs)in photocatalytic hydrogen peroxide(H_(2)O_(2))production.SACs offer multiple benefits over traditional catalysts such as improved efficiency,selectivity,and flexibility due to their distinct electronic structure and unique properties.The review discusses the critical elements in the design of SACs,including the choice of metal atom,host material,and coordination environment,and how these elements impact the catalytic activity.The role of single atoms in photocatalytic H_(2)O_(2)production is also analysed,focusing on enhancing light absorption and charge generation,improving the migration and separation of charge carriers,and lowering the energy barrier of adsorption and activation of reactants.Despite these advantages,several challenges,including H_(2)O_(2)decomposition,stability of SACs,unclear mechanism,and low selectivity,need to be overcome.Looking towards the future,the review suggests promising research directions such as direct utilization of H_(2)O_(2),high-throughput synthesis and screening,the creation of dual active sites,and employing density functional theory for investigating the mechanisms of SACs in H_(2)O_(2)photosynthesis.This review provides valuable insights into the potential of single atom catalysts for advancing the field of photocatalytic H_(2)O_(2)production.

Single atom gold catalysts for low-temperature CO oxidation

Low‐temperature CO oxidation is important for both fundamental studies and practical applica‐tions. Supported gold catalysts are generally regarded as the most active catalysts for low‐temperature CO oxidation. The active sites are traditionally believed to be Au nanoclusters or nanoparticles in the size range of 0.5–5 nm. Only in the last few years have single‐atom Au catalysts been proved to be active for CO oxidation. Recent advances in both experimental and theoretical studies on single‐atom Au catalysts unambiguously demonstrated that when dispersed on suitable oxide supports the Au single atoms can be extremely active for CO oxidation. In this mini‐review, recent advances in the development of Au single‐atom catalysts are discussed, with the aim of illus‐trating their unique catalytic features during CO oxidation.