https://scholars.lib.ntu.edu.tw/handle/123456789/638489
Title: | Reversibly Adapting Configuration in Atomic Catalysts Enables Efficient Oxygen Electroreduction | Authors: | Tan, Hui-Ying Lin, Sheng-Chih Wang, Jiali Chen, Jui-Hsien Chang, Chia-Jui Hou, Cheng-Hung Shyue, Jing-Jong Kuo, Tsung-Rong HAO MING CHEN |
Issue Date: | 13-Dec-2023 | Journal Volume: | 145 | Journal Issue: | 49 | Start page/Pages: | 27054 | Source: | Journal of the American Chemical Society | Abstract: | Single-atom catalysts (SACs) featuring M-N-C moieties have garnered significant attention as efficient electrocatalysts for the oxygen reduction reaction (ORR). However, the role of the dynamic M-N configuration of SACs induced by the derived frameworks under applied ORR potentials remains poorly understood. Herein, we conduct a comprehensive investigation using multiple operando techniques to assess the dynamic configurations of Cu SACs under various microstructural interface (MSI) regulations by anchoring atomic Cu on g-C3N4 and zeolitic imidazolate framework (ZIF) substrates. Cu SACs supported on g-C3N4 exhibit symmetric Cu-N configurations characterized by a reversibly adaptive nature under operational conditions, which leads to their excellent ORR catalytic activity. In contrast, the Cu-N configuration in ZIF-derived Cu SACs undergoes irreversible structural changes during the ORR process, in which the elongated Cu-N pair is unstable and breaks during the ORR, acting as a competing reaction against the ORR and resulting in high overpotential requirements. Crucially, operando time-resolved X-ray absorption spectroscopy (TR-XAS) and Raman results unequivocally reveal the reversibly adapting properties of the local Cu-N configuration in atomic Cu-anchored g-C3N4, which have been overlooked in numerous literatures. All findings provide valuable insights into the potential-driven characteristics of atomic electrocatalysts during target reactions and offer a systematic approach to study atomic electrocatalysts and their corresponding catalytic behaviors. |
URI: | https://scholars.lib.ntu.edu.tw/handle/123456789/638489 | ISSN: | 00027863 | DOI: | 10.1021/jacs.3c10707 |
Appears in Collections: | 化學系 |
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