Fa Dejuan, Yuan Jiangyan, Feng Guangyuan, Lei Shengbin, Hu Wenping
Tianjin Key Laboratory of Molecular Optoelectronic Science, Department of Chemistry, School of Science & Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin University, Tianjin, 300072, P. R. China.
Angew Chem Int Ed Engl. 2023 Apr 24;62(18):e202300532. doi: 10.1002/anie.202300532. Epub 2023 Mar 9.
Bimetallic electrocatalysts with its superior performance has a broad application prospect in oxygen evolution reaction (OER), but the fundamental understanding of the mechanism of synergistic effect is still limited since there lacks a practical way to decouple the influence factors on the intrinsic activity of active sites from others. Herein, a series of bimetallic Co-Ni two-dimensional polymer (2DP) model OER catalysts with well-defined architecture, monolayer characteristic, were designed and synthesized to explore the influence of the coupling strength between metal centers on OER performance. The coupling strength was regulated by adjusting the spacing between metal centers or the conjugation degree of bridge skeleton. Among the examined 2DPs, CoTAPP-Ni-MF-2DP, which has the strongest coupling strength between metal centers exhibited the best OER performance. These model systems can help to explore the precise structure-performance relationships, which is important for the rational catalyst design at the atomic/molecular levels.
具有优异性能的双金属电催化剂在析氧反应（OER）中具有广阔的应用前景，但由于缺乏一种实用的方法来将影响活性位点本征活性的因素与其他因素解耦，对协同效应机制的基本理解仍然有限。在此，设计并合成了一系列具有明确结构、单层特征的双金属Co-Ni二维聚合物（2DP）模型OER催化剂，以探索金属中心之间的耦合强度对OER性能的影响。通过调整金属中心之间的间距或桥连骨架的共轭程度来调节耦合强度。在所研究的2DP中，金属中心之间耦合强度最强的CoTAPP-Ni-MF-2DP表现出最佳的OER性能。这些模型体系有助于探索精确的结构-性能关系，这对于原子/分子水平上的合理催化剂设计至关重要。
