Surface-exposed single-Ni atoms with potential-driven dynamic behaviors for highly efficient electrocatalytic oxygen evolution
Trapping the active sites on the exterior surface of hollow supports can reduce mass transfer resistance and enhance atomic utilization. Herein, we report a facile chemical vapor deposition strategy to synthesize single-Ni atoms decorated hollow S/N-doped football-like carbon spheres (Ni SAs@S/N-FCS...
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sg-ntu-dr.10356-1661232023-06-21T08:19:47Z Surface-exposed single-Ni atoms with potential-driven dynamic behaviors for highly efficient electrocatalytic oxygen evolution Zhao, Yafei Lu, Xue Feng Fan, Guilan Luan, Deyan Gu, Xiaojun Lou, David Xiong Wen School of Chemical and Biomedical Engineering School of Chemistry, Chemical Engineering and Biotechnology Science::Chemistry Electrocatalysis· Hollow S/N-Doped Carbon Spheres Trapping the active sites on the exterior surface of hollow supports can reduce mass transfer resistance and enhance atomic utilization. Herein, we report a facile chemical vapor deposition strategy to synthesize single-Ni atoms decorated hollow S/N-doped football-like carbon spheres (Ni SAs@S/N-FCS). Specifically, the CdS@3-aminophenol/formaldehyde is carbonized into S/N-FCS. The gas-migrated Ni species are anchored on the surface of S/N-FCS simultaneously, yielding Ni SAs@S/N-FCS. The obtained catalyst exhibits outstanding performance for alkaline oxygen evolution reaction (OER) with an overpotential of 249 mV at 10 mA cm−2, a small Tafel slope of 56.5 mV dec−1, and ultra-long stability up to 166 hours without obvious fading. Moreover, the potential-driven dynamic behaviors of Ni-N4 sites and the contribution of the S dopant at different locations in the matrix to the OER activity are revealed by the operando X-ray absorption spectroscopy and theoretical calculations, respectively. Ministry of Education (MOE) Submitted/Accepted version X.W.L. acknowledges the funding support from the Ministry of Education of Singapore through the Academic Research Fund (AcRF) Tier-2 grant (MOE2019-T2-2-049). X.J.G. acknowledges the funding support from the National Natural Science Foundation of China (22162019), and the Science and Technology Projects of Inner Mongolia Autonomous Region (2021GG0195). 2023-04-17T08:43:41Z 2023-04-17T08:43:41Z 2022 Journal Article Zhao, Y., Lu, X. F., Fan, G., Luan, D., Gu, X. & Lou, D. X. W. (2022). Surface-exposed single-Ni atoms with potential-driven dynamic behaviors for highly efficient electrocatalytic oxygen evolution. Angewandte Chemie International Edition, 61(45), e202212542-. https://dx.doi.org/10.1002/anie.202212542 1433-7851 https://hdl.handle.net/10356/166123 10.1002/anie.202212542 45 61 e202212542 en MOE2019-T2-2-049 Angewandte Chemie International Edition © 2022 Wiley-VCHGmbH. All rights reserved. This is the peer reviewed version of the following article: Zhao, Y., Lu, X. F., Fan, G., Luan, D., Gu, X. & Lou, D. X. W. (2022). Surface-exposed single-Ni atoms with potential-driven dynamic behaviors for highly efficient electrocatalytic oxygen evolution. Angewandte Chemie International Edition, 61(45), e202212542-, which has been published in final form at https://doi.org/10.1002/anie.202212542. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions. application/pdf |
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Science::Chemistry Electrocatalysis· Hollow S/N-Doped Carbon Spheres Zhao, Yafei Lu, Xue Feng Fan, Guilan Luan, Deyan Gu, Xiaojun Lou, David Xiong Wen Surface-exposed single-Ni atoms with potential-driven dynamic behaviors for highly efficient electrocatalytic oxygen evolution |
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Trapping the active sites on the exterior surface of hollow supports can reduce mass transfer resistance and enhance atomic utilization. Herein, we report a facile chemical vapor deposition strategy to synthesize single-Ni atoms decorated hollow S/N-doped football-like carbon spheres (Ni SAs@S/N-FCS). Specifically, the CdS@3-aminophenol/formaldehyde is carbonized into S/N-FCS. The gas-migrated Ni species are anchored on the surface of S/N-FCS simultaneously, yielding Ni SAs@S/N-FCS. The obtained catalyst exhibits outstanding performance for alkaline oxygen evolution reaction (OER) with an overpotential of 249 mV at 10 mA cm−2, a small Tafel slope of 56.5 mV dec−1, and ultra-long stability up to 166 hours without obvious fading. Moreover, the potential-driven dynamic behaviors of Ni-N4 sites and the contribution of the S dopant at different locations in the matrix to the OER activity are revealed by the operando X-ray absorption spectroscopy and theoretical calculations, respectively. |
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School of Chemical and Biomedical Engineering |
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School of Chemical and Biomedical Engineering Zhao, Yafei Lu, Xue Feng Fan, Guilan Luan, Deyan Gu, Xiaojun Lou, David Xiong Wen |
format |
Article |
author |
Zhao, Yafei Lu, Xue Feng Fan, Guilan Luan, Deyan Gu, Xiaojun Lou, David Xiong Wen |
author_sort |
Zhao, Yafei |
title |
Surface-exposed single-Ni atoms with potential-driven dynamic behaviors for highly efficient electrocatalytic oxygen evolution |
title_short |
Surface-exposed single-Ni atoms with potential-driven dynamic behaviors for highly efficient electrocatalytic oxygen evolution |
title_full |
Surface-exposed single-Ni atoms with potential-driven dynamic behaviors for highly efficient electrocatalytic oxygen evolution |
title_fullStr |
Surface-exposed single-Ni atoms with potential-driven dynamic behaviors for highly efficient electrocatalytic oxygen evolution |
title_full_unstemmed |
Surface-exposed single-Ni atoms with potential-driven dynamic behaviors for highly efficient electrocatalytic oxygen evolution |
title_sort |
surface-exposed single-ni atoms with potential-driven dynamic behaviors for highly efficient electrocatalytic oxygen evolution |
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2023 |
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https://hdl.handle.net/10356/166123 |
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1772826297638060032 |