Jia Shuaiqiang, Zhu Qinggong, Wu Haihong, Han Shitao, Chu Mengen, Zhai Jianxin, Xing Xueqing, Xia Wei, He Mingyuan, Han Buxing
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University Shanghai 200062 China
Institute of Eco-Chongming 20 Cuiniao Road, ChenjiaTown, Chongming District Shanghai 202162 China.
Chem Sci. 2022 Jun 10;13(25):7509-7515. doi: 10.1039/d1sc06964k. eCollection 2022 Jun 29.
Use of multi-metallic catalysts to enhance reactions is an interesting research area, which has attracted much attention. In this work, we carried out the first work to prepare trimetallic electrocatalysts by a one-step co-electrodeposition process. A series of Cu-X-Y (X and Y denote different metals) catalysts were fabricated using this method. It was found that CuLaCs (the content ratio of Cu, La, and Cs in the electrolyte is 10 : 1 : 1 in the deposition process), which had an elemental composition of CuLaCs in the catalyst, formed a composite structure on three dimensional (3D) carbon paper (CP), which showed outstanding performance for CO electroreduction reaction (CORR) to produce ethylene (CH). The faradaic efficiency (FE) of CH could reach 56.9% with a current density of 37.4 mA cm in an H-type cell, and the partial current density of CH was among the highest ones up to date, including those over the catalysts consisting of Cu and noble metals. Moreover, the FE of C products (CH, ethanol, and propanol) over the CuLaCs catalyst in a flow cell reached 70.5% with a high current density of 486 mA cm. Experimental and theoretical studies suggested that the doping of La and Cs into Cu could efficiently enhance the reaction efficiency a combination of different effects, such as defects, change of electronic structure, and enhanced charge transfer rate. This work provides a simple method to prepare multi-metallic catalysts and demonstrates a successful example for highly efficient CORR using non-noble metals.
使用多金属催化剂来增强反应是一个有趣的研究领域,已引起了广泛关注。在这项工作中,我们首次通过一步共电沉积法制备了三金属电催化剂。采用该方法制备了一系列Cu-X-Y(X和Y表示不同金属)催化剂。研究发现,CuLaCs(在沉积过程中,电解质中Cu、La和Cs的含量比为10∶1∶1)在催化剂中具有CuLaCs的元素组成,在三维(3D)碳纸(CP)上形成了复合结构,在将CO电还原反应(CORR)生成乙烯(CH)方面表现出优异的性能。在H型电解池中,CH的法拉第效率(FE)可达56.9%,电流密度为37.4 mA cm ,CH的分电流密度是迄今为止最高的之一,包括那些在由Cu和贵金属组成的催化剂上的分电流密度。此外,在流动电解池中,CuLaCs催化剂上C产物(CH、乙醇和丙醇)的FE在高电流密度486 mA cm 时达到70.5%。实验和理论研究表明,将La和Cs掺杂到Cu中可以有效地提高反应效率,这是不同效应的组合,如缺陷、电子结构变化和电荷转移速率提高。这项工作提供了一种制备多金属催化剂的简单方法,并展示了使用非贵金属进行高效CORR的成功实例。