Zhou Chong, Zhang Rui, Rong Youwen, Yang Yaoyue, Jiang Xiaole
Key Laboratory of Fundamental Chemistry of the State Ethnic Commission, School of Chemistry and Environment, Southwest Minzu University, Chengdu 610041, China.
State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China.
ACS Appl Mater Interfaces. 2023 Sep 13;15(36):42585-42593. doi: 10.1021/acsami.3c08187. Epub 2023 Aug 30.
The reasonable design of atomically dispersed Ni-N sites in porous carbon nanostructures is an efficient strategy to enhance the electrochemical CO reduction reaction (CORR) catalytic activity. In this work, atomically dispersed Ni-N sites on hierarchically porous carbon catalysts (HP-Ni-NC) were fabricated by a facile NaCl template-assisted pyrolysis method. The catalysts exhibit a large specific surface area and a hierarchical porous structure, facilitating the exposure of numerous active sites and the mass/electron transport during the CORR. Consequently, the CO Faradaic efficiency maintained over 90% in a wide potential window on the optimized HP-Ni-NC-2 catalyst. The CO partial current achieved 15.2 mA cm at -0.9 V (vs reversible hydrogen electrode) in a H-cell. Furthermore, the current density can achieve 250 mA cm at a cell voltage of 3.11 V in a membrane electrode assembly electrolyzer, demonstrating great promise for commercial-scale application. This study presents a facile approach to synthesizing hierarchically porous structure single-atom catalysts with superior catalytic performance toward CORR.
在多孔碳纳米结构中合理设计原子分散的Ni-N位点是提高电化学CO还原反应（CORR）催化活性的有效策略。在这项工作中，通过简便的NaCl模板辅助热解方法制备了分级多孔碳催化剂（HP-Ni-NC）上的原子分散Ni-N位点。这些催化剂具有大的比表面积和分级多孔结构，有利于在CORR过程中暴露大量活性位点以及促进质量/电子传输。因此，在优化的HP-Ni-NC-2催化剂上，CO法拉第效率在宽电位窗口内保持在90%以上。在H型电解池中，-0.9 V（相对于可逆氢电极）时CO分电流达到15.2 mA cm²。此外，在膜电极组件电解槽中，电池电压为3.11 V时电流密度可达到250 mA cm²，显示出在商业规模应用中的巨大潜力。本研究提出了一种简便的方法来合成对CORR具有优异催化性能的分级多孔结构单原子催化剂。
