Institution: | 1. 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;2. 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;3. Shanghai Synchrotron Radiation Facility, Zhangjiang Lab, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201210 Shanghai, P.?R. China;4. Department of Polymer Materials, School of Materials Science and Engineering, Shanghai University, 200444 Shanghai, P.?R. China |
Abstract: | Electrochemical synthesis of H2O2 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 H2O2 directly from O2 and H2O. The precise-designed MgP-DHTA-COF achieves H2O2 selectivity up to 96%, high Faradaic efficiency of 91% and reliable stability for H2O2 synthesis in 0.10 mol L?1 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 H2O2 production. |