Wang Mengjun, Dong Xu, Meng Zhaodong, Hu Zhiwei, Lin Yan-Gu, Peng Chun-Kuo, Wang Hongshuai, Pao Chih-Wen, Ding Songyuan, Li Youyong, Shao Qi, Huang Xiaoqing
State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China.
College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Jiangsu, 215123, China.
Angew Chem Int Ed Engl. 2021 May 10;60(20):11190-11195. doi: 10.1002/anie.202100897. Epub 2021 Apr 8.
Two-dimensional (2D) metal-organic framework nanosheets (MOF NSs) play a vital role in catalysis, but the most preparation is ultrasonication or solvothermal. Herein, a liquid-liquid interfacial synthesis method has been developed for the efficient fabrication of a series of 2D Ni MOF NSs. The active sites could be modulated by readily tuning the ratios of metal precursors and organic linkers (R ). The Ni MOF NSs display highly R dependent activities towards 2e oxygen reduction reaction (ORR) to hydrogen peroxide (H O ), where the Ni MOF NSs with the R of 6 exhibit the optimal near-zero overpotential, ca. 98 % H O selectivity and production rate of ca. 80 mmol g h in 0.1 M KOH. As evidenced by X-ray absorption fine structure spectroscopy, the coordination environment of active sites changed from saturation to unsaturation, and the partially unsaturated metal atoms are crucial to create optimal sites for enhancing the electrocatalysis.
二维（2D）金属有机框架纳米片（MOF NSs）在催化中起着至关重要的作用，但大多数制备方法是超声处理或溶剂热法。在此，已开发出一种液 - 液界面合成方法用于高效制备一系列二维镍金属有机框架纳米片。通过轻松调节金属前驱体与有机连接体的比例（R），活性位点可以得到调控。镍金属有机框架纳米片对2e氧还原反应（ORR）生成过氧化氢（H₂O₂）表现出高度依赖于R的活性，其中R为6的镍金属有机框架纳米片表现出最佳的近零过电位，约98%的H₂O₂选择性和约80 mmol g⁻¹ h⁻¹的产率，在0.1 M KOH中。如X射线吸收精细结构光谱所证明的，活性位点的配位环境从饱和变为不饱和，部分不饱和的金属原子对于创建增强电催化的最佳位点至关重要。
