High Atom Utilization Efficiency Research Articles

Multifunctional molecular precursor with tunable nano-microarchitecture enables exceptional electromagnetic waves absorption

Multi-component carbon is a promising candidate for electromagnetic wave (EMW) absorption materials. However, complex and non-green preparation process with low atomic utilization efficiency compromises the merits of carbon materials. Additionally, enhancing the electromagnetic wave absorption (EMWA) is highly desirable. To face the challenge, a multifunctional molecular precursor (DQSDCI) has been developed, characterized by high atom utilization efficiency (high char yield), abundant in-situ nitrogen doping, multi-sites for composite of nano-materials (e.g. CNT) or metal ion (e.g. iron) and green preparation (water solubility). The multi-component carbons derived from DQSDCI, featuring adjustable nanostructures (nanoribbons or nanosheets) and modifiable porosity, demonstrate outstanding EMWA. The multicomponent carbon of DQSDCI, iron and CNT (DQSDCI-Fe-CNT-700) demonstrated a minimum reflection loss (RLmin) of −69.57 dB and a maximum effective absorption bandwidth (EABmax) of 5.7 GHz at about 2 mm thickness, covering a wide frequency range (4–18 GHz) by controlling the thickness between 1 and 5 mm. Moreover, simulation results indicated that the derived nanosheet is very promising application for aircraft stealth in a monostatic radar system. Abundant in-situ N doping, uniform distribution of MWCNT and ferromagnetic nanoparticles, hierarchical pore structures and various heterogeneous interfaces can synergistically improve the EMW attenuation ability by forming optimal impedance matching and multi-polarization loss.

Fluorine-Tuned Carbon-Based Nickel Single-Atom Catalysts for Scalable and Highly Efficient CO2 Electrocatalytic Reduction.

Electrocatalytic CO2 reduction is garnering significant interest due to its potential applications in mitigating CO2 and producing fuel. However, the scaling up of related catalysis is still hindered by several challenges, including the cost of the catalytic materials, low selectivity, small current densities to maintain desirable selectivity. In this study, Fluorine (F) atoms were introduced into an N-doped carbon-supported single nickel (Ni) atom catalyst via facile polymer-assisted pyrolysis. This method not only maintains the high atom utilization efficiency of Ni in a cost-effective and sustainable manner but also effectively manipulates the electronic structure of the active Ni-N4 site through F doping. The catalyst has also been further optimized by controlling the F states, including convalent and semi-ionic states, by adjusting the fluorine sources involved. Consequently, this catalyst with unique structure exhibited comparable electrocatalytic performance for CO2-to-CO conversion, achieving a Faradaic efficiency (FE) of over 99% across a wide potential range and an exceptional CO evolution rate of 9.5 × 104 h-1 at -1.16 V vs reversible hydrogen electrode (RHE). It also delivered a practical current of 400 mA cm-2 while maintaining more than 95% CO FE. Experimental analysis combined with density functional theory (DFT) calculations have also shown that F-doping modifies the electron configuration at the central Ni-N4 sites. This modification lowers the energy barrier for CO2 activation, thereby facilitating the production of the crucial *COOH intermediate.

Sulfur Modified Carbon-Based Single-Atom Catalysts for Electrocatalytic Reactions.

Efficient and sustainable energy development is a powerful tool for addressing the energy and environmental crises. Single-atom catalysts (SACs) have received high attention for their extremely high atom utilization efficiency and excellent catalytic activity, and have broad application prospects in energy development and chemical production. M-N4 is an active center model with clear catalytic activity, but its catalytic properties such as catalytic activity, selectivity, and durability need to be further improved. Adjustment of the coordination environment of the central metal by incorporating heteroatoms (e.g., sulfur) is an effective and feasible modification method. This paper describes the precise synthetic methods for introducing sulfur atoms into M-N4 and controlling whether they are directly coordinated with the central metal to form a specific coordination configuration, the application of sulfur-doped carbon-based single-atom catalysts in electrocatalytic reactions such as ORR, CO2RR, HER, OER, and other electrocatalytic reaction are systematically reviewed. Meanwhile, the effect of the tuning of the electronic structure and ligand configuration parameters of the active center due to doped sulfur atoms with the improvement of catalytic performance is introduced by combining different characterization and testing methods. Finally, several opinions on development of sulfur-doped carbon-based SACs are put forward.

Accelerating the design of catalysts for CO2 electroreduction to HCOOH: A data-driven DFT-ML screening of dual atom catalysts

Dual-atom catalysts (DACs) have emerged as potential catalysts for effective electroreduction of CO2 due to their high atom utilization efficiency and multiple active sites. However, the screening of DACs remains a challenge due to the large number of possible combinations, making exhaustive experimental or computational screening a daunting task. In this study, a density functional theory (DFT)-based machine learning (ML)-accelerated (DFT-ML) hybrid approach was developed to test a set of 406 dual transition metal catalysts on N-doped graphene (NG) for the electroreduction of CO2 to HCOOH. The results showed that the ML algorithms can successfully capture the relationship between the descriptors of the DACs (inputs) and the limiting potential for HCOOH generation (output). Of the four ML algorithms studied in this work, the feedforward neural network model achieved the highest prediction accuracy (the highest correlation coefficient (R2) of 0.960 and the lowest root mean square error (RMSE) of 0.319 eV on the test set) and the predicted results were verified by DFT calculations with an average absolute error of 0.14 eV. The DFT-ML approach identified Co-Co-NG and Ir-Fe-NG as the most active and stable electrocatalysts for the electrochemical reduction of CO2 to HCOOH. The DFT-ML hybrid approach exhibits exceptional prediction accuracy while enabling a significant reduction in screening time by an impressive 64% compared to conventional DFT-only calculations. These results demonstrate the immense potential of using ML methods to accelerate the screening and rational design of efficient catalysts for various energy and environmental applications.

Machine Learning-Assisted Study of RENxC6-x-Doped Graphene as Potential Electrocatalysts for Oxygen Electrode Reactions.

In the application of renewable energy, the oxidation-reduction reaction (ORR) and oxygen evolution reaction (OER) are two crucial reactions. Single-atom catalysts (SACs) based on metal-doped graphene have been widely employed due to their high activity and high atom utilization efficiency. However, the catalytic activity is significantly influenced by different metals and local coordination, making it challenging to efficiently screen through either experimental or density functional theory (DFT) calculations. To address this issue, this study employed a combination of DFT calculations and machine learning (DFT-ML) to investigate rare earth-modified carbon-based (RENxC6-x) electrocatalysts. Based on computational data from 75 catalysts, we trained two ML models to capture the underlying patterns of physical properties and overpotential. Subsequently, the candidate catalysts were screened, leading to the discovery of four ORR catalysts, nine OER catalysts, and five bifunctional electrocatalysts, all of which were thoroughly validated for their stability. Lastly, by integrating the ML models with the SHAP analysis framework, we revealed the influence of atomic radius, Pauling electronegativity, and other features on the catalytic activity. Additionally, we analyzed the physicochemical properties of potential catalysts through DFT calculations. The revolutionary DFT-ML approach provides a crucial driving force for the design and synthesis of potential catalysts in subsequent studies.

Non-noble metal single-atoms for oxygen electrocatalysis in rechargeable zinc-air batteries: recent developments and future perspectives.

Ever-growing demands for zinc-air batteries (ZABs) call for the development of advanced electrocatalysts. Single-atom catalysts (SACs), particularly those for isolating non-noble metals (NBMs), are attracting great interest due to their merits of low cost, high atom utilization efficiency, structural tunability, and extraordinary activity. Rational design of advanced NBM SACs relies heavily on an in-depth understanding of reaction mechanisms. To gain a better understanding of the reaction mechanisms of oxygen electrocatalysis in ZABs and guide the design and optimization of more efficient NBM SACs, we herein organize a comprehensive review by summarizing the fundamental concepts in the field of ZABs and the recent advances in the reported NBM SACs. Moreover, the selection of NBM elements and supports of SACs and some effective strategies for enhancing the electrochemical performance of ZABs are illustrated in detail. Finally, the challenges and future direction in this field of ZABs are also discussed.

Transition metal oxide clusters: advanced electrocatalysts for a sustainable energy future.

The comprehensive utilization of sustainable green energy is essential to face the global energy and environmental crisis. The oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and electrocatalytic urea synthesis (EUS) are the pivotal electrocatalytic processes, necessitating the development of low-cost electrocatalysts with high efficiency. Small-sized transition metal oxide (TMO) clusters have attracted a lot of attention because of their exceptional qualities, such as exhibiting a dense array of low-coordinated metal active sites (e.g. abundant metal cation defects and oxygen vacancy), amorphous structures with high surface energy, high atom utilization efficiency, and cost-effectiveness. Furthermore, the synergistic actions between metal clusters and TM-Nx single atom active sites remarkably boost up the electrocatalytic performances, corroborated by density functional theory (DFT). More efforts in this comprehensive feature article are expected to achieve insights into the fundamental understanding of electrocatalytic reaction mechanisms in our lab and serve as a guide for creating cutting-edge electrocatalysts of transition metal oxide clusters.

Atomically dispersed dinuclear iridium active sites for efficient and stable electrocatalytic chlorine evolution reaction.

The electrochemical chlorine evolution reaction (CER) is a critical anode reaction in chlor-alkali electrolysis. Although precious metal-based mixed metal oxides (MMOs) have long been used as CER catalysts, they suffer from high cost and poor selectivity due to the competing oxygen evolution reaction (OER). Single-atom catalysts (SACs), featuring high atom utilization efficiency, have captured widespread interest in diverse applications. However, the single-atom sites in SACs are generally recognized as independent motifs and the interplay of adjacent sites is largely overlooked. Herein, we report a "precursor-preselected" cage-encapsulated strategy to synthesize atomically dispersed dinuclear iridium active sites bridged by oxygen that are supported on nitrogen-doped carbon (Ir2-ONC). The dinuclear Ir2-ONC catalyst exhibits a CER onset potential of 1.375 V vs. normal hydrogen electrode, a high faradaic efficiency of >95%, and a high mass activity of 14321.6 A gIr -1, much better than the Ir SACs, which demonstrates the significance of coordination and electronic structure regulation for atomically dispersed catalysts. Density functional theory calculations and ab initio molecular dynamics simulations confirm that the unique dinuclear structure facilitates Cl- adsorption, resulting in improved catalytic CER performance.

Single-atom Fe nanozymes with excellent oxidase-like and laccase-like activity for colorimetric detection of ascorbic acid and hydroquinone.

Although traditional Fe-based nanozymes have shown great potential, generally only a small proportion of the Fe atoms on the catalyst's surface are used. Herein, we synthesized single-atom Fe on N-doped graphene nanosheets (Fe-CNG) with high atom utilization efficiency and a unique coordination structure. Active oxygen species including superoxide radicals (O2•-) and singlet oxygen (1O2) were efficiently generated from the interaction of the Fe-CNG with dissolved oxygen in acidic conditions. The Fe-CNG nanozymes were found to display enhanced oxidase-like and laccase-like activity, with Vmax of 2.07 × 10-7M∙S-1 and 4.54 × 10-8M∙S-1 and Km of 0.324mM and 0.082mM, respectively, which is mainly due to Fe active centers coordinating with O and N atoms simultaneously. The oxidase-like performance of the Fe-CNG can be effectively inhibited by ascorbic acid (AA) or hydroquinone (HQ), which can directly obstruct the oxidation of 3,3',5,5'-tetramethylbenzidine (TMB). Therefore, a direct and sensitive colorimetric method for the detection of AA and HQ activity was established, which exhibited good linear detection and limit of detection (LOD) of 0.048μM and 0.025μM, respectively. Moreover, a colorimetric method based on the Fe-CNG catalyst was fabricated for detecting the concentration of AA in vitamin C. Therefore, this work offers a new method for preparing a single-atom catalyst (SAC) nanozyme and a promising strategy for detecting AA and HQ.

Single-Atom-Based Oxygen Reduction Reaction Catalysts for Proton Exchange Membrane Fuel Cells: Progress and Perspective.

Single-atom catalysts (SACs) are regarded as promising non-noble-metal alternatives for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells due to their high atom utilization efficiency and excellent catalytic properties. However, the insufficient long-term stability issues of SACs under the working conditions seriously hinder their practical application. In this perspective, the recent progress of SACs with optimized ORR catalytic activity is first reviewed. Then, the possible degradation mechanisms of SACs in the ORR process and effective strategies for improving their ORR durability are summarized. Finally, some challenges and opportunities are proposed to develop stable single-atom-based ORR electrocatalysts in the future.

Loading IrOx Clusters on MnO2 Boosts Acidic Water Oxidation via Metal-Support Interaction.

Noble metal-based electrocatalysts are crucial for efficient acidic water oxidation to develop green hydrogen energy. However, traditional noble metal catalysts loaded on inactive substrates show limited intrinsic catalytic activity, and their large sizes have compromised the atom efficiency of these noble metals. Herein, IrOx nanoclusters with sizes below 2 nm, displaying high atom-utilization efficiency of Ir species, were supported on a redox-active MnO2 nanosubstrate (IrOx/MnO2) with different phases (α-MnO2, δ-MnO2, and ε-MnO2) to explore the optimal combination. Electrochemical measurements showed that IrOx/ε-MnO2 had excellent OER performance with a low overpotential of 225 mV at 10 mA cm-2 in 0.5 M H2SO4, superior to its counterpart, IrOx/α-MnO2 (242 mV) and IrOx/δ-MnO2 (286 mV). Moreover, it also delivered robust stability with no obvious change in operating potential at 10 mA cm-2 during 50 h of continuous operation. Combining the XPS results and Bader charge analysis, we demonstrated that the strong metal-support interactions of IrOx/ε-MnO2 could effectively regulate the electronic structures of the active Ir atoms and stabilize IrOx nanoclusters on supports to suppress their detachment, resulting in significantly enhanced catalytic activity and stability for acidic OER. DFT calculations further supported that the enhanced catalytic OER performance of IrOx/ε-MnO2 could be ascribed to the appropriate strength of interactions between the active Ir sites and the reaction intermediates of the potential-determining step (*O and *OOH) regulated by the redox-active substrates.

Size and Synergy Effects of Ultrafine 2.6 nm CoNi Nanoparticles Within 3D Crisscross N‐Doped Porous Carbon Nanosheets for Efficient Water Splitting

AbstractA non‐precious metal‐based catalyst for water electrolysis provides great promise for cost‐effective and highly efficient sustainable hydrogen production. It herein rationally synthesizes uniform superminiature CoNi nanoparticles (2.6 nm) embedded in 3D N‐doped randomly oriented and erected porous carbon nanosheets (CoNi@N‐PCNS). Taking advantage of the large specific surface area, expedited intermediate transport, and effectively exposed active sites of the hierarchical architecture, located CoNi nanoparticles yield a high atom utilization efficiency. Density functional theory calculations indicate that synergetic and cooperative interactions inside CoNi alloy modulate the d‐band center, leading to a moderate adsorption and desorption energy of reaction intermediates, further accelerating both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) kinetics. Accordingly, the as‐synthesized CoNi@N‐PCNS catalyst establishes superb catalytic activities for HER and OER, revealing overpotentials of 71.2 and 263.8 mV at 10 mA cm−2, respectively. Remarkably, when assembled as a two‐electrode electrolyzer, a satisfying cell voltage of 1.59 V at 10 mA cm−2, and superior stability are demonstrated, highlighting great promise toward water electrolysis.

Atomic Layers of B2 CuPd on Cu Nanocubes as Catalysts for Selective Hydrogenation.

The search for highly active and selective catalysts with high precious metal atom utilization efficiency has attracted increasing interest in both the fundamental synthesis of materials and important industrial reactions. Here, we report the synthesis of Pd-Cu nanocubes with a Cu core and an ordered B2 intermetallic CuPd shell with controllable atomic layers on the surface (denoted as Cu/B2 CuPd), which can efficiently and robustly catalyze the selective hydrogenation of acetylene (C2H2) to ethylene (C2H4) under mild conditions. The optimized Cu/B2 CuPd with a Pd loading of 9.5 at. % exhibited outstanding performance in the C2H2 semi-hydrogenation with 100% C2H2 conversion and 95.2% C2H4 selectivity at 90 °C. We attributed this outstanding performance to the core/shell structure with a high surface density of active Pd sites isolated by Cu in the B2 intermetallic matrix, representing a structural motif of single-atom alloys (SAAs) on the surface. The combined experimental and computational studies further revealed that the electronic states of Pd and Cu are modulated by SAAs from the synergistic effect between Pd and Cu, leading to enhanced performance compared with pristine Pd and Cu catalysts. This study provides a new synthetic methodology for making single-atom catalysts with high precious metal atom utilization efficiency, enabling simultaneous tuning of both geometric and electronic structures of Pd active sites for enhanced catalysis.

Rapid synthesis of Palladium-Platinum-Nickel ultrathin porous nanosheets with high catalytic performance for alcohol electrooxidation

Bimetallic two-dimensional (2D) nanomaterials are widely used in electrocatalysis owing to their unique physicochemical properties, while trimetallic 2D materials of porous structures with large surface area are rarely reported. In this paper, a one-pot hydrothermal synthesis of ternary ultra-thin PdPtNi nanosheets is developed. By adjusting the volume ratio of the mixed solvents, PdPtNi with porous nanosheets (PNSs) and ultrathin nanosheets (UNSs) was prepared. The growth mechanism of PNSs was investigated through a series of control experiments. Notably, thanks to the high atom utilization efficiency and fast electron transfer, the PdPtNi PNSs have remarkable activity of methanol oxidation reaction (MOR) and ethanol oxidation reaction (EOR). The mass activities of the well-tuned PdPtNi PNSs for MOR and EOR were 6.21 A mg−1 and 5.12 A mg−1, respectively, much higher than those of commercial Pt/C and Pd/C. In addition, after durability test, the PdPtNi PNSs exhibited desirable stability with the highest retained current density. Therefore, this work provides a significant guidance for designing and synthesizing a new 2D material with excellent catalytic performance toward direct fuel cells applications.

Advances in Transition-Metal-Based Dual-Atom Oxygen Electrocatalysts.

Oxygen electrocatalysis has aroused considerable interest over the past years because of the new energy technologies boom in hydrogen energy and metal-air battery. However, due to the sluggish kinetic of the four-electron transfer process in oxygen reduction reaction and oxygen evolution reaction, the electro-catalysts are urgently needed to accelerate the oxygen electrocatalysis. Benefit from the high atom utilization efficiency, unprecedentedly high catalytic activity, and selectivity, single-atom catalysts (SACs) are considered the most promising candidate to replace the traditional Pt-group-metal catalysts. Compared with SACs, the dual-atom catalysts (DACs) are attracting more attraction including higher metal loading, more versatile active sites, and excellent catalytic activity. Therefore, it is essential to explore the new universal methods approaching to the preparation, characterization, and to elucidate the catalytic mechanisms of the DACs. In this review, several general synthetic strategies and structural characterization methods of DACs are introduced and the involved oxygen catalytic mechanisms are discussed. Moreover, the state-of-the-art electrocatalytic applications including fuel cells, metal-air batteries, and water splitting have been sorted out at present. The authors hope this review has given some insights and inspiration to the researches about DACs in electro-catalysis.

Pd/Co Catalyst with High Pd Atom Utilization Efficiency for Nitrobenzene Hydrogenation at Room Temperature: Experimental and DFT Studies.

Enhancing catalytic performance as well as reducing catalyst cost are the eternal pursuit for the catalysis community. Herein, a simple and effective palladium-doped cobalt (Pd/Co) catalyst with high Pd atom utilization efficiency was synthesized via galvanic replacement reaction for the selective hydrogenation of nitrobenzene with H2 at room temperature, delivering >99 % yield of aniline with up to 158 times higher catalytic activity than commercial palladium powder. Detailed characterizations and DFT calculations revealed that Co-Pd interaction leads to a decrease in electron density of Pd and the distance between Pd atoms that results in the enhanced catalytic performance. Further experiments indicated that the Pd/Co catalyst serves as a highly efficient, selective, and recyclable catalyst for a range of nitroarene substrates. This work might provide a green and sustainable methodology to design and synthesize highly active catalysts with high utilization efficiency of the noble metals in fundamental and applied research.

Surface synergistic effect of sub-2 nm NiFeCr hydroxide nanodots yielding high oxygen evolution mass activities

Designing cost-effective electrocatalysts with high efficiency and stability for oxygen evolution reaction (OER) is crucial for hydrogen generation by water splitting and meta-air batteries. NiFe catalysts doped with transition-metal cations have offered an efficient approach to tuning the atomic and electronic structure, thus enhancing OER activity. However, most research focused on regulating the composition of atoms in large-sized catalysts, which remains a major challenge to achieving high atom utilization efficiency and optimal surface synergistic effect. Herein, a one-step co-precipitation method is presented to directly synthesize ultrafine NiFeCr trimetallic amorphous hydroxide nanodots (AND-NiFeCr, < 2 nm) to fully expose the atoms at the surface and near-surface region. Electronic-structure investigation revealed a strong synergistic electronic interaction between Ni, Fe, and Cr cations, which subtly tailors ternary catalysts' local atomic and electronic configuration. Due to the refined ultrafine nano- and electronic-structure modulation, the optimized AND-NiFeCr (Ni:Fe:Cr = 5:3:2) catalysts demonstrated superior OER activity with a low overpotential of 271 mV at 10 mA cm−2. Moreover, an extraordinarily high mass activity of 4926 A gMetal-1 at the overpotential of 300 mV was achieved. This work provides a novel surface synergistic effect strategy to design highly efficient NiFe-based ultrafine hydroxide OER catalysts with high atomic utilization efficiency.

A 2D/2D heterojunction of ultrathin Pd nanosheet/MXene towards highly efficient methanol oxidation reaction: the significance of 2D material nanoarchitectonics.

Two-dimensional (2D) Pd nanosheet-based catalysts have recently garnered widespread attention due to their high atom utilization efficiency. However, their catalytic ability and structural stability still require significant enhancement before they can be widely applied. In this study, we presented the rational design and controllable fabrication of a novel 2D/2D heterojunction, which consists of ultrathin Pd nanosheets (NSs) grown on the Ti3C2Tx MXene surface (Pd NSs/MXene). This heterostructure was achieved through a robust and convenient stereo-assembly strategy. The newly developed Pd NSs/MXene heterojunction not only provides numerous exposed active Pd atoms with an optimized electronic structure but also enables an intimate Pd/MXene interfacial interaction, ensuring a stable hybrid configuration. Consequently, the resulting Pd NSs/MXene heterojunction exhibits exceptional methanol oxidation properties. It possesses a large electrochemically active surface area, high mass and specific activities, and a long operating life, which are significantly superior to those of traditional Pd nanoparticle/carbon and Pd nanosheet/carbon catalysts. Theoretical simulations further reveal strong electronic interactions between the Pd nanosheet and MXene, which dramatically enhance the adsorption energy of the Pd component and simultaneously lower its d-band center. As a result, the Pd NSs/MXene heterojunction is less susceptible to CO poisoning. This work introduces a new 2D/2D heterojunction based on MXene and noble metallic materials and holds significance for the development of other novel heterojunctions, particularly within the realm of 2D material nanoarchitectonics.

Pt Single Atoms on CrN Nanoparticles Deliver Outstanding Activity and CO Tolerance in the Hydrogen Oxidation Reaction.

The large-scale application of proton exchange membrane fuel cells is currently hampered by high cost of commercial Pt catalysts and their susceptibility to poisoning by CO impurities in H2 feed. In this context, the development of CO-tolerant electrocatalysts with high Pt atom utilization efficiency for hydrogen oxidation reaction (HOR) is of critical importance. Herein, Pt single atoms are successfully immobilized on chromium nitride nanoparticles by atomic layer deposition method, denoted as Pt SACs/CrN. Electrochemical tests establish Pt SACs/CrN to be a very efficient HOR catalyst, with a mass activity that is 5.7 times higher than commercial PtRu/C. Strikingly, the excellent performance of Pt SACs/CrN is maintained after introducing 1000ppm of CO in H2 feed. The excellent CO-tolerance of Pt SACs/CrN is related to weaker CO adsorption on Pt single atoms. This work provides guidelines for the design and construction of active and CO-tolerant catalysts for HOR.

Strong Electronic Metal-Support Interaction between Iridium Single Atoms and a WO3 Support Promotes Highly Efficient and Robust CO2 Cycloaddition.

The carbon dioxide (CO2 ) cycloaddition of epoxides to cyclic carbonates is of great industrial importance owing to the high economical values of its products. Single-atom catalysts (SACs) have great potential in CO2 cycloaddition by virtue of their high atom utilization efficiency and desired activity, but they generally suffer from poor reaction stability and catalytic activity arising from the weak interaction between the active centers and the supports. In this work, Ir single atoms stably anchored on the WO3 support (Ir1 -WO3 ) are developed with a strong electronic metal-support interaction (EMSI). Superior CO2 cycloaddition is realized in the Ir1 -WO3 catalyst via the EMSI effect: 100% conversion efficiency for the CO2 cycloaddition of styrene oxide to styrene carbonate after 15h at 40 °C and excellent stability with no degradation even after ten reaction cycles for a total of more than 150h. Density functional theory calculations reveal that the EMSI effect results in significant charge redistribution between the Ir single atoms and the WO3 support, and consequently lowers the energy barrier associated with epoxide ring opening. This work furnishes new insights into the catalytic mechanism of CO2 cycloaddition and would guide the design of stable SACs for efficient CO2 cycloaddition reactions.