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Effective Descriptor for Nitrogen Reduction on Atomic Catalysts

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Abstract

Single- and bi-atom catalysts (SACs and BACs) exhibit great potential in catalyzing electrochemical nitrogen reduction reaction (NRR) due to their unusual coordination-environment effect of active centers, which unfortunately remains elusive so far. Herein, by applying a descriptor ψ based on the valence-electron number and electronegativity of the catalytic centers, we have systematically studied NRR on SACs and BACs with diverse coordination environments. Our results quantify the elemental type and number of metal atoms and their neighbors at the active centers on the adsorption properties and reactivity of atomic catalysts. This uncovers the pronounced differences and similarities between SACs, homonuclear BACs, and heteronuclear BACs as well as the unique role of N dopant. With these findings, we have also predicted that Ir-N4-SAC and TiMn-N6-BAC as promising candidates for further experimental studies. Therefore, our findings can serve as useful guidelines for developing high-performance catalysts for NRR.

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Acknowledgements

The authors are thankful for the support from the National Natural Science Foundation of China (Nos. 21673095, 51631004, 11974128, 51702345 and 22173034), the Opening Project of State Key Laboratory of High Performance Ceramics and Superfine Microstructure (SKL201910SIC), the Program of Innovative Research Team (in Science and Technology) in University of Jilin Province, the Program for JLU (Jilin University) Science and Technology Innovative Research Team (No. 2017TD-09), the Fundamental Research Funds for the Central Universities, the Shanghai Natural Science Foundation of China (21ZR1472900) and the computing resources of the High Performance Computing Center of Jilin University.

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  1. School of Materials Science and Engineering, Jilin University, Changchun, 130022, China

    Xin Liu & Wang Gao

  2. State Key Laboratory of Applied Optics, Changchun Institute of Optics, Fine Mechanics and Physics, Chinese Academy of Sciences, No.3888 Dong Nanhu Road, Changchun, 130033, China

    Liujian Qi

  3. State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 1295 Dingxi Road, Shanghai, 200050, China

    Erhong Song

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  1. Xin Liu
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Liu, X., Qi, L., Song, E. et al. Effective Descriptor for Nitrogen Reduction on Atomic Catalysts. Catal Lett 153, 300–310 (2023). https://doi.org/10.1007/s10562-022-03979-4

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