文献类型：期刊文献

英文题名：Enhancing CO2 Electroreduction with Au/Pyridine/Carbon Nanotubes Hybrid Structures

作者：Ma, Zhongqiao[1];Lian, Cheng[1];Niu, Dongfang[1];Shi, Lei[1];Hu, Shuozhen[1];Zhang, Xinsheng[1];Liu, Honglai[1]

机构：[1]East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China

年份：2019

卷号：12

期号：8

起止页码：1724

外文期刊名：CHEMSUSCHEM

收录：;EI(收录号：20191406729187);WOS:【SCI-EXPANDED(收录号:WOS:000466387800019)】；

基金：We acknowledge the National Key R&D Program of China (2017YFB0307502 and 2017YFB0307500), the 111 Project of China (B08021), the Collaborative Innovation Centre for Petrochemical New Materials, Anqing, Anhui, P. R. China (246011), and the Shanghai Pujiang Program (18PJ1402000). We also thank the Research Center of Analysis and Test of East China University of Science and Technology for help with the characterization.

语种：英文

外文关键词：carbon dioxide; density function calculations; electrocatalysis; gold; reactive intermediates

摘要：Selective electrochemical reduction of CO2 by using renewable electricity has received considerable attention because of the potential to convert a harmful greenhouse gas into useful chemicals. A high-performance electrocatalyst for CO2 reduction is constructed based on metal nanoparticles/organic molecule hybrid materials. On the nanoscale, Au nanoparticles are uniformly anchored on carbon nanotubes to afford substantially increased current density, improved selectivity for CO, and enhanced stability. On the molecular level, the catalytic performance is further enhanced by introducing axial pyridine groups to the surface of the carbon nanotubes. The resulting hybrid catalyst exhibits around 93 % faradaic efficiency for CO production over a wide potential range (-0.58 to -0.98 V), a high mass activity of 251 A g(Au)(-1) at -0.98 V in aqueous solution at near-neutral pH, and strong stability with continuous electrolysis for 10 h at -0.58 V. DFT calculations indicate that the synergistic effects of Au and axial pyridine could dramatically stabilize the key intermediate (*COOH) formed in the rate-limiting step of CO2 reduction, which effectively lowers the overpotential.