一种用于增强水氧化催化的异常稳定的基于八钴簇的金属有机框架。

Huang Ning-Yu, Shen Jian-Qiang, Ye Zi-Ming, Zhang Wei-Xiong, Liao Pei-Qin, Chen Xiao-Ming

MOE Key Laboratory of Bioinorganic and Synthetic Chemistry , School of Chemistry , Sun Yat-Sen University , Guangzhou 510275 , China . Email:

Department of Chemical and Biomolecular Engineering , University of California , Los Angeles , CA 90095 , USA.

Chem Sci. 2019 Sep 10;10(42):9859-9864. doi: 10.1039/c9sc03224j. eCollection 2019 Nov 14.

Extensive efforts have been devoted to developing efficient and durable catalysts for water oxidation. Herein, we report a highly stable metal-organic framework that shows high catalytic activity and durability for electrically driven (an overpotential of 430 mV at 10 mA cm in neutral aqueous solution) and photodriven (a turnover frequency of 16 s and 12 000 cycles) water oxidation, representing the best catalyst for water oxidation reported to date. Computational simulation and isotope tracing experiments showed that the μ-OH group of the {Co(μ-OH)} unit participates in the water oxidation reaction to offer an oxygen vacancy site with near-optimal OH adsorption energy.

人们已经付出了巨大努力来开发用于水氧化的高效且耐用的催化剂。在此，我们报道了一种高度稳定的金属有机框架，它在电驱动（在中性水溶液中，10 mA cm² 时过电位为 430 mV）和光驱动（周转频率为 16 s⁻¹ 且循环次数为 12000 次）水氧化反应中表现出高催化活性和耐久性，是迄今为止报道的用于水氧化的最佳催化剂。计算模拟和同位素示踪实验表明，{Co(μ-OH)}单元的μ-OH基团参与水氧化反应，提供了一个具有近乎最佳OH吸附能的氧空位位点。