文献类型：期刊文献

英文题名：Engineering the Ni-N-C Catalyst Microenvironment Enabling CO2 Electroreduction with Nearly 100% CO Selectivity in Acid

作者：Sheng, Xuedi[1];Ge, Wangxing[2];Jiang, Hongliang[1];Li, Chunzhong[1,2]

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

年份：2022

卷号：34

期号：38

外文期刊名：ADVANCED MATERIALS

收录：;EI(收录号：20223512630279);WOS:【SCI-EXPANDED(收录号:WOS:000842804000001)】；

基金：This work was supported by the National Natural Science Foundation of China (21838003, 91834301, 21978278, and 21978087), the Shanghai Scientific and Technological Innovation Project (18JC1410500 and 19JC1410400), and the Fundamental Research Funds for the Central Universities (222201718002). The authors thank the Shanghai Synchrotron Radiation Facility (14W1, SSRF), the Beijing Synchrotron Radiation Facility (1W1B and soft-X-ray endstation, BSRF), and the Hefei Synchrotron Radiation Facility (Photoemission, Magnetic Circular Dichroism and Catalysis/Surface Science Endstations, Endstations at National Synchrotron Radiation Laboratory).

语种：英文

外文关键词：carbon dioxide electroreduction; electrocatalysis; gas-diffusion electrodes; structure engineering; working microenvironment

摘要：CO2 electrolysis in acid has emerged as a promising route to achieve high CO2 utilization due to the inhibition of undesired carbonate formation that generally occurs in alkaline or neutral conditions. However, the efficiency and stability of this system need to be further improved through tailoring of the electrocatalyst and its working environment. Here, a working microenvironment of structurally engineered Ni-N-C catalyst for acidic CO2 electrolysis is probed and optimized by adding hydrophobic poly(tetrafluoroethylene) (PTFE) nanoparticles in the catalytic layer of gas-diffusion electrodes. The PTFE-modified electrode delivers nearly 100% CO Faradaic efficiency at an industry-relevant current density of 250 mA cm(-2), and a high single-pass CO2 utilization of 75.7% at a current density of 200 mA cm(-2) under 20 sccm CO2 gas flow rate. Moreover, compared to a conventional electrode without added PTFE, the PTFE-modified electrode exhibits a substantially enhanced water-flooding-resistant ability. Mechanistic investigations reveal that a moderate PTFE modification can optimize the local CO2/H2O ratio in the catalytic layer, favoring the reduction of the diffusion layer thickness and the formation of a highly active and stable solid-liquid-gas interfacial microenvironment.