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Enhancing CO 2 Electroreduction with Au/Pyridine/Carbon Nanotubes Hybrid Structures
Author(s) -
Ma Zhongqiao,
Lian Cheng,
Niu Dongfang,
Shi Lei,
Hu Shuozhen,
Zhang Xinsheng,
Liu Honglai
Publication year - 2019
Publication title -
chemsuschem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 2.412
H-Index - 157
eISSN - 1864-564X
pISSN - 1864-5631
DOI - 10.1002/cssc.201802940
Subject(s) - overpotential , electrocatalyst , carbon nanotube , faraday efficiency , catalysis , materials science , electrolysis , electrochemistry , chemical engineering , nanoparticle , selectivity , electrochemical reduction of carbon dioxide , aqueous solution , inorganic chemistry , nanotechnology , chemistry , organic chemistry , electrode , carbon monoxide , engineering , electrolyte
Selective electrochemical reduction of CO 2 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 CO 2 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 CO 2 reduction, which effectively lowers the overpotential.