Modulating the local coordination environment of single-atom catalysts for enhanced catalytic performance

Li, Xinyuan; Rong, Hongpan; Zhang, Jiatao; Wang, Dingsheng; Li, Yadong

doi:10.1007/s12274-020-2755-3

Cited by 608 publications

(340 citation statements)

References 132 publications

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“…In summary, the coordination environment of the single atoms in SACs, including the coordinated atoms, coordination numbers and the second‐ and high‐coordination shell, has a significant effect on the microscopic properties and catalytic performances of SACs. [ 97 ] To precisely control the coordination environment of SACs by elaborated synthetic methods and to elucidate the surroundings of SACs by advanced characterization techniques are of great importance to increase the catalytic performance and unveil the structure‐activity relationship of SACs.…”

Section: Fundamentals Of the Co2rr On Sacsmentioning

confidence: 99%

Heterogeneous Single‐Atom Catalysts for Electrochemical CO₂ Reduction Reaction

et al. 2020

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The electrochemical CO2 reduction reaction (CO2RR) is of great importance to tackle the rising CO2 concentration in the atmosphere. The CO2RR can be driven by renewable energy sources, producing precious chemicals and fuels, with the implementation of this process largely relying on the development of low‐cost and efficient electrocatalysts. Recently, a range of heterogeneous and potentially low‐cost single‐atom catalysts (SACs) containing non‐precious metals coordinated to earth‐abundant elements have emerged as promising candidates for the CO2RR. Unfortunately, the real catalytically active centers and the key factors that govern the catalytic performance of these SACs remain ambiguous. Here, this ambiguity is addressed by developing a fundamental understanding of the CO2RR‐to‐CO process on SACs, as CO accounts for the major product from CO2RR on SACs. The reaction mechanism, the rate‐determining steps, and the key factors that control the activity and selectivity are analyzed from both experimental and theoretical studies. Then, the synthesis, characterization, and the CO2RR performance of SACs are discussed. Finally, the challenges and future pathways are highlighted in the hope of guiding the design of the SACs to promote and understand the CO2RR on SACs.

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Section: Fundamentals Of the Co2rr On Sacsmentioning

confidence: 99%

Heterogeneous Single‐Atom Catalysts for Electrochemical CO₂ Reduction Reaction

et al. 2020

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“…In fact, modulating the local coordination environment of transition-metal single atoms has been demonstrated as an effective way in tuning their catalytic activity, selectivity and stability. [99][100][101][102] In a latest work, our group pinpointed FeCO as an efficient H 2 O 2 Figure 5. Recently developed transition metal single atoms doped carbon materials for 2e − ORR.…”

Section: Defects and Heteroatoms Engineering On Carbon-based Catalystsmentioning

confidence: 99%

Catalyst Design for Electrochemical Oxygen Reduction toward Hydrogen Peroxide

Jiang

Zhao

Wang

2020

Adv Funct Materials

217

107

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Precise electrochemical synthesis under ambient conditions has provided emerging opportunities for renewable energy utilization. Among many promising systems, the production of hydrogen peroxide (H2O2) from the cathodic oxygen reduction reaction (ORR) has attracted considerable interest in past decades due to the increasing market demands and the vital role of ORR in the electrocatalysis field. This work describes recent advances in cathodic materials for H2O2 synthesis from 2e- ORR. By using Pt as a stereotype, the tuning knobs are overviewed, including the intrinsic binding strength of oxygenated species, the intermediate diffusion path and the isolation of Pt–Pt ensembles that enable 2e- ORR pathway from 4e- total reduction. This knowledge is successfully applied to other transition metal systems and leads to the discovery of more efficient alloy catalysts with balanced improvement on both activity and selectivity. In addition, mesostructure engineering and heteroatoms doping strategies on carbon‐based materials, which significantly boost the H2O2 production efficiency as compared to intact carbon sites, are also reviewed. Finally, future directions and challenges of transferring developed catalysts from lab scale tests to pilot plant operations are briefly outlooked.

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“…[12][13][14][15][16][17][18][19][20] Meanwhile, many potential applications are explored. [21][22][23][24][25][26][27][28][29][30][31] However, some challenges still remain in the research direction of SAS catalysts. On one hand, the reported synthetic methods and unexpected catalytic performances of such catalysts are still the tip of the iceberg.…”

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confidence: 99%

Gram‐Scale Synthesis of High‐Loading Single‐Atomic‐Site Fe Catalysts for Effective Epoxidation of Styrene

et al. 2020

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Single‐atomic‐site (SAS) catalysts, a new frontier of catalysts, always show extremely high atom efficiency and unexpected catalytic properties. Herein, a pyrolyzing coordinated polymer (PCP) strategy is developed, which is facile and widely applicable in the synthesis of a series of SAS catalysts including SAS‐Fe, SAS‐Ni, SAS‐Cu, SAS‐Zn, SAS‐Ru, SAS‐Rh, SAS‐Pd, SAS‐Pt, and SAS‐Ir. The as‐obtained SAS catalysts can be easily synthesized at gram scale and the metal loading of SAS‐Fe catalysts achieves a record value of 30 wt%, which meets the requirement of practical applications. Moreover, it is discovered that SAS‐Fe catalysts show unprecedented catalytic performance for epoxidation of styrene using O2 as the only oxidant (yield: 64%; selectivity: 89%), while Fe nanoparticles and ironporphyrin are inactive. This discovery is believed to pave the way for exploiting the unparalleled properties of SAS catalysts and promoting their industrial applications.

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Modulating the local coordination environment of single-atom catalysts for enhanced catalytic performance

Cited by 608 publications

References 132 publications

Heterogeneous Single‐Atom Catalysts for Electrochemical CO₂ Reduction Reaction

Heterogeneous Single‐Atom Catalysts for Electrochemical CO₂ Reduction Reaction

Catalyst Design for Electrochemical Oxygen Reduction toward Hydrogen Peroxide

Gram‐Scale Synthesis of High‐Loading Single‐Atomic‐Site Fe Catalysts for Effective Epoxidation of Styrene

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Modulating the local coordination environment of single-atom catalysts for enhanced catalytic performance

Cited by 608 publications

References 132 publications

Heterogeneous Single‐Atom Catalysts for Electrochemical CO2 Reduction Reaction

Heterogeneous Single‐Atom Catalysts for Electrochemical CO2 Reduction Reaction

Catalyst Design for Electrochemical Oxygen Reduction toward Hydrogen Peroxide

Gram‐Scale Synthesis of High‐Loading Single‐Atomic‐Site Fe Catalysts for Effective Epoxidation of Styrene

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Product

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Heterogeneous Single‐Atom Catalysts for Electrochemical CO₂ Reduction Reaction

Heterogeneous Single‐Atom Catalysts for Electrochemical CO₂ Reduction Reaction