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| Pàgina inicial > Articles > Articles publicats > Electron delocalization engineering via hierarchical modulation in single-atom catalysts for highly efficient electrochemical CO2 reduction |
(Institut Català de Nanociència i Nanotecnologia) (Chinese Academy of Sciences) (East China University of Science and Technology) (Institut de Recerca en Energia de Catalunya) (Chinese Academy of Sciences) (Ernst Ruska-Centre for Microscopy and Spectroscopy with Electrons (Jülich, Alemanya)) (Max-Planck-Institutfur Eisenforschung GmbH) (Institut Català de Nanociència i Nanotecnologia) (Ernst Ruska-Centre for Microscopy and Spectroscopy with Electrons (Jülich, Alemanya)) (Institució Catalana de Recerca i Estudis Avançats) (Aarhus University) (Universitat de Barcelona. Departament de Física) (Institut Català de Nanociència i Nanotecnologia) (Institut Català de Nanociència i Nanotecnologia)
| Data: | 2025 |
| Resum: | Modulating the coordination of atomically dispersed MN moieties to enhance electron asymmetry presents a promising strategy for improving catalytic performance in the electrochemical reduction of carbon dioxide (eCORR). By combining small amounts of Au nanoclusters with lateral oxygen coordination in the first coordination shell, the enhanced electron delocalization on Ni centers improves both activity and selectivity. Experimentally, the optimized catalyst demonstrates exceptional catalytic performance, achieving over 95% Faradaic efficiency (FE) for CO across a broad potential range from - 0. 50 to - 0. 85 V vs. RHE. It also achieves over 90% FE for CO at an overpotential of 340 mV, outperforming state-of-the-art Ni-based single-atom catalysts (SACs). Moreover, the catalyst shows promising potential at a higher current density (∼150 mA cm) in a flow cell, maintaining high CO selectivity (over 90%). Structural characterizations and theoretical calculations indicate that this structure enhances electron redistribution around Ni sites through a unique electron tug effect. This effectively stabilizes *COOH intermediates, favoring CO production during eCORR at low applied potentials. This work offers a valuable method that extends beyond the first coordination shell, augmenting the complexity of electronic distribution on metal centers, which could be adapted for further fine-tuning the catalytic behavior of SACs in various reactions. |
| Ajuts: | Generalitat de Catalunya 2021/SGR-00457 Generalitat de Catalunya 2021/SGR-01581 Agencia Estatal de Investigación PRTR-C17.I1 Agencia Estatal de Investigación PID2023-149158OB-C43 Agencia Estatal de Investigación CEX2021-001214-S European Commission 101146498 European Commission 101105092 |
| Nota: | Altres ajuts: CERCA Programme/Generalitat de Catalunya |
| Drets: | Aquest document està subjecte a una llicència d'ús Creative Commons. Es permet la reproducció total o parcial, la distribució, la comunicació pública de l'obra i la creació d'obres derivades, fins i tot amb finalitats comercials, sempre i quan es reconegui l'autoria de l'obra original.  |
| Llengua: | Anglès |
| Document: | Article ; recerca ; Versió publicada |
| Matèria: | Single atom catalysts ; Electron tug effect ; CO2 electroreduction ; High CO selectivity ; Wide potential range ; Au nanoclusters |
| Publicat a: | Chemical engineering journal, Vol. 507 (March 2025) , art. 160634, ISSN 1385-8947 |
