Guo Yu, Xu Qing, Yang Shuai, Jiang Zheng, Yu Chengbing, Zeng Gaofeng
Department of Polymer Materials, School of Materials Science and Engineering, Shanghai University, 200444, Shanghai, P. R. China.
CAS Key Laboratory of Low-Carbon Conversion Science and Engineering, Shanghai Advanced Research Institute (SARI), Chinese Academy of Sciences (CAS), 201210, Shanghai, P. R. China.
Chem Asian J. 2021 Mar 1;16(5):498-502. doi: 10.1002/asia.202100030. Epub 2021 Jan 22.
Electrochemical synthesis of H O with high productivity is a significant challenge in electrocatalysis. Herein, we develop Mg-ion contained covalent organic frameworks (MgP-DHTA-COF), comprising stacked 2D layers, well-defined skeletons, and well-ordered monodispersed active sites, for the electrocatalytic production of H O directly from O and H O. The precise-designed MgP-DHTA-COF achieves H O selectivity up to 96%, high Faradaic efficiency of 91% and reliable stability for H O synthesis in 0.10 mol L KOH aqueous solution. Both experiments and simulations demonstrate that the pyrrolic-N fixed Mg ions in the knots promote the reactivity of COF and enhance the adsorption ability of OOH*. This work provides a valuable example for the design of an efficient electrocatalyst based on COFs for H O production.
通过电化学合成高效生产过氧化氢是电催化领域的一项重大挑战。在此，我们开发了含镁离子的共价有机框架（MgP-DHTA-COF），其由堆叠的二维层、明确的骨架和有序的单分散活性位点组成，用于直接从氧气和水进行电催化生产过氧化氢。精心设计的MgP-DHTA-COF在0.10 mol·L的氢氧化钾水溶液中实现了高达96%的过氧化氢选择性、91%的高法拉第效率以及过氧化氢合成的可靠稳定性。实验和模拟均表明，节点中吡咯氮固定的镁离子促进了共价有机框架的反应活性，并增强了超氧羟基自由基（OOH*）的吸附能力。这项工作为设计基于共价有机框架的高效过氧化氢生产电催化剂提供了一个有价值的范例。
