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Title: | Orbital coupling of hetero-diatomic nickel-iron site for bifunctional electrocatalysis of CO₂ reduction and oxygen evolution | Authors: | Zeng, Zhiping Gan, Liyong Yang, Hongbin Su, Xiaozhi Gao, Jiajian Liu, Wei Matsumoto, Hiroaki Gong, Jun Zhang, Junming Cai, Weizhen Zhang, Zheye Yan, Yibo Liu, Bin Chen, Peng |
Keywords: | Engineering::Chemical engineering | Issue Date: | 2021 | Source: | Zeng, Z., Gan, L., Yang, H., Su, X., Gao, J., Liu, W., Matsumoto, H., Gong, J., Zhang, J., Cai, W., Zhang, Z., Yan, Y., Liu, B. & Chen, P. (2021). Orbital coupling of hetero-diatomic nickel-iron site for bifunctional electrocatalysis of CO₂ reduction and oxygen evolution. Nature Communications, 12(1), 4088-. https://dx.doi.org/10.1038/s41467-021-24052-5 | Project: | A1983c0025 A20E5c0080 MOE2017-T2-2- 005 MOET2EP10120-0002 RG4/20 |
Journal: | Nature Communications | Abstract: | While inheriting the exceptional merits of single atom catalysts, diatomic site catalysts (DASCs) utilize two adjacent atomic metal species for their complementary functionalities and synergistic actions. Herein, a DASC consisting of nickel-iron hetero-diatomic pairs anchored on nitrogen-doped graphene is synthesized. It exhibits extraordinary electrocatalytic activities and stability for both CO2 reduction reaction (CO2RR) and oxygen evolution reaction (OER). Furthermore, the rechargeable Zn-CO2 battery equipped with such bifunctional catalyst shows high Faradaic efficiency and outstanding rechargeability. The in-depth experimental and theoretical analyses reveal the orbital coupling between the catalytic iron center and the adjacent nickel atom, which leads to alteration in orbital energy level, unique electronic states, higher oxidation state of iron, and weakened binding strength to the reaction intermediates, thus boosted CO2RR and OER performance. This work provides critical insights to rational design, working mechanism, and application of hetero-DASCs. | URI: | https://hdl.handle.net/10356/172407 | ISSN: | 2041-1723 | DOI: | 10.1038/s41467-021-24052-5 | Schools: | School of Chemistry, Chemical Engineering and Biotechnology School of Chemical and Biomedical Engineering |
Rights: | © 2021 The Author(s). This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/ licenses/by/4.0/. | Fulltext Permission: | open | Fulltext Availability: | With Fulltext |
Appears in Collections: | CCEB Journal Articles |
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