文献类型：期刊文献

英文题名：Low full-cell voltage driven high-current-density selective paired formate electrosynthesis

作者：Xiao, Chuqian[1];Cheng, Ling[2];Wang, Yating[1];Liu, Jinze[2];Chen, Rongzhen[1];Jiang, Hao[1];Li, Yuhang[1];Li, Chunzhong[1,2]

机构：[1]East China Univ Sci & Technol, Sch Mat Sci & Engn, Frontiers Sci & Ctr Mat & Dynam Chem, Key Lab Ultrafine Mat Minist Educ Shanghai Engn R, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Sch Chem Engn, Shanghai 200237, Peoples R China

年份：2022

卷号：10

期号：3

起止页码：1329

外文期刊名：JOURNAL OF MATERIALS CHEMISTRY A

收录：;EI(收录号：20220511558470);WOS:【SCI-EXPANDED(收录号:WOS:000731739300001)】；

基金：This work was supported by the National Natural Science Foundation of China (22178104, 21838003, 91834301, and 22008069), the Shanghai Scientific and Technological Innovation Project (18JC1410500 and 19JC1410400), the Innovation Program of Shanghai Municipal Education Commission, "the Fundamental Research Funds for the Central Universities", and the Shanghai Sailing Program (20YF1410200).

语种：英文

外文关键词：Current density - Methanol - Carbon dioxide - Coordination reactions - Cobalt alloys - Anodic oxidation - Electrocatalysis - Electrocatalysts - Binary alloys

摘要：Anodic selective electro-oxidation of methanol paired with cathodic carbon dioxide (CO2) reduction is regarded as a promising strategy to generate value-added formate products. We first design a 3D-assembled NiCo layered double hydroxide electrocatalyst containing sulfur with a low coordination number (S-NiCo-LDH) for methanol oxidation to formate. We decrease the anodic methanol-to-formate working potential to 1.39 V (vs. RHE) at 100 mA cm(-2), and maintain similar to 100% formate faradaic efficiency at a high current density up to 300 mA cm(-2) with >60 mV, lower than the previous best potentials in the literature. From the remaining S 2p(1/2) peak after electrocatalysis, we demonstrate that the low-coordinated sulfur on the catalyst surface serves as the promoter for the reaction. In the end, when combining the CO2 reduction in the cathode, we achieve a record low full-cell voltage of 2.48 V to drive selective paired formate electrosynthesis at a high current density of 300 mA cm(-2).