Research Article

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2021, 14(9): 3234–3239

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https://doi.org/10.1007/s12274-021-3315-1

Working-in-tandem mechanism of multi-dopants in enhancing electrocatalytic nitrogen reduction reaction performance of carbonbased materials

Wenqing Zhang1, Keke Mao2, Jingxiang Low1, Hengjie Liu1, Yanan Bo1, Jun Ma1, Qiaoxi Liu1, Yawen Jiang1, Jiuzhong Yang1, Yang Pan1, Zeming Qi1, Ran Long1 (✉), Li Song1, and Yujie Xiong1,3 (✉)

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1 Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), School of Chemistry and Materials Science, and National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230041, China
2 School of Energy and Environment Science, Anhui University of Technology, Maanshan 243032, China
3 Institute of Energy, Hefei Comprehensive National Science Center, Hefei 230031, China

Keywords: N2 reduction reaction, metal-free catalyst, heteroatoms doping, asymmetric charge distribution, electrocatalysis
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  • Abstract
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Developing carbon-based electrocatalysts with excellent N2 adsorption and activation capability holds the key to achieve highly efficient nitrogen reduction reaction (NRR) for reaching its practical application. Here, we report a highly active electrocatalyst— metal-free pyrrolic-N dominated N, S co-doped carbon (pyrr-NSC) for NRR. Based on theoretical and experimental results, it is confirmed that the N and S-dopants practice a working-in-tandem mechanism on pyrr-NSC, where the N-dopants are utilized to create electropositive C sites for enhancing N2 adsorption and the S-dopants are employed to induce electron backdonation for facilitating N2 activation. The synergistic effect of the pyrrolic-N and S-dopants can also suppress the irritating hydrogen evolution reaction, further boosting the NRR performance. This work gives an indication that the combination of two different dopants on electrocatalyst can enhance NRR performance by working in the two tandem steps—the adsorption and activation of N2 molecules, providing a new strategy for NRR electrocatalyst design.
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Working-in-tandem mechanism of multi-dopants in enhancing electrocatalytic nitrogen reduction reaction performance of carbonbased materials. Nano Res. 2021, 14(9): 3234–3239 https://doi.org/10.1007/s12274-021-3315-1

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