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Single-Atom Catalysts: Advances and Challenges in Metal-Support Interactions for Enhanced Electrocatalysis

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Abstract

Single-atom catalysts (SACs), which contain a single metal atom supported on a well-confined substrate, are among the most promising heterogeneous catalysts owing to their unique advantages, such as high intrinsic activity and selectivity, tunable bonds and coordination, abundant metal-containing active sites, and atomic economy. Since metal-support interactions (MSIs) in SACs exert a substantial influence on the catalytic properties, gaining a profound understanding and recognition of catalytic reactions depends greatly on investigating MSIs both experimentally and computationally. Hence, the engineering and modulation of MSIs are regarded as one of the most efficient methods to rationally design SACs with disruptively enhanced catalytic properties. In this review, we track the recent advances in SACs from an MSI perspective. We then discuss the existing MSIs in SACs and elucidate the significant role of strong MSIs in catalytic properties and mechanisms. The challenges hindering the rational design of supported SACs with strong MSIs, which are currently still far from being completely understood and overcome, are described. In addition, the correlation between strong MSIs and electrocatalytic activities in SACs, including an outlook to increase our understanding of MSIs, is discussed. Finally, the present review provides some perspectives and an in-depth understanding of strong MSIs to advance high-performing SACs.

Graphic Abstract

Metal-support interaction (MSI) in single metal atom catalysts (SMACs) is vital for regulating catalytic properties, including oxygen- and hydrogen-involving electrocatalytic reactions.

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Copyright© 2019, Springer Nature. Reproduced with permission. b Changes in the band structure followed by an increased number of Ce4+ ions per Cu site. Reprinted with permission from Ref. [40]. Copyright© 2020, Springer Nature. Reproduced with permission

Fig. 5

Copyright© 2018, American Chemical Society. Reproduced with permission. b The process of photogenerated electron excitation, transformation and localization. Reprinted with permission from Ref. [68]. Copyright© 2019, Springer Nature. Reproduced with permission. c Au SAs prefer to disperse and stabilize on step sites of CeO2 rather than terrace surfaces. Reprinted with permission from Ref. [69]. Copyright© 2017, American Chemical Society. Reproduced with permission

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Copyright© 2018, Springer Nature. Reproduced with permission

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Copyright© 2020, Royal Society of Chemistry. Reproduced with permission

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Copyright© 2020, John Wiley & Sons, Inc. Reproduced with permission

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Copyright© 2019, John Wiley & Sons, Inc. Reproduced with permission

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Copyright© 2020, Elsevier. Reproduced with permission. b, c Reaction free energy on two edge-N atoms (PtN2) and two carbon atoms (PtC2) and the chemical state of the corresponding intermediate. Reprinted with permission from Ref. [175]. Copyright© 2019, Springer Nature. Reproduced with permission

Fig. 11

Copyright© 2018, Springer Nature. Reproduced with permission. c–e CoN2+2 and CoN4 active moieties for the 4e− ORR pathway (c) and corresponding reaction free energy (d) and chemical state (e). CoN2+2 is the more favorable configuration after comparison. Reprinted with permission from Ref. [188]. Copyright © 2019, Royal Society of Chemistry. Reproduced with permission

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Copyright© 2016, Springer Nature. Reproduced with permission

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Reproduced with permission from Ref [213], Wiley-VCH (2017). b Schematic showing the preparation of Co, Fe SA-coordinated N-doped carbon. Reprinted with permission from Ref. [214]. American Chemical Society (2017)

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Copyright© 2019, American Association for the Advancement of Science. Reproduced with permission

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Acknowledgements

This work was partially supported by the National Natural Science Foundation of China (Grant No. 21771030) and the Natural Science Foundation of Liaoning Province (2020-MS-113).

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  1. School of Chemical Engineering, Dalian University of Technology, Dalian, 116024, Liaoning, China

    Yang Mu, Changgong Meng & Yifu Zhang

  2. State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan, 430070, Hubei, China

    Tingting Wang & Zongkui Kou

  3. School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan, 430074, Hubei, China

    Jian Zhang

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Mu, Y., Wang, T., Zhang, J. et al. Single-Atom Catalysts: Advances and Challenges in Metal-Support Interactions for Enhanced Electrocatalysis. Electrochem. Energy Rev. 5, 145–186 (2022). https://doi.org/10.1007/s41918-021-00124-4

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