Electrokinetic and in situ spectroscopic investigations of CO electrochemical reduction on copper

Jing Li, Xiaoxia Chang, Haochen Zhang, Arnav S. Malkani, Mu jeng Cheng, Bingjun Xu, Qi Lu

研究成果: Article同行評審

1 引文 斯高帕斯(Scopus)

摘要

Rigorous electrokinetic results are key to understanding the reaction mechanisms in the electrochemical CO reduction reaction (CORR), however, most reported results are compromised by the CO mass transport limitation. In this work, we determined mass transport-free CORR kinetics by employing a gas-diffusion type electrode and identified dependence of catalyst surface speciation on the electrolyte pH using in-situ surface enhanced vibrational spectroscopies. Based on the measured Tafel slopes and reaction orders, we demonstrate that the formation rates of C2+ products are most likely limited by the dimerization of CO adsorbate. CH4 production is limited by the CO hydrogenation step via a proton coupled electron transfer and a chemical hydrogenation step of CO by adsorbed hydrogen atom in weakly (7 < pH < 11) and strongly (pH > 11) alkaline electrolytes, respectively. Further, CH4 and C2+ products are likely formed on distinct types of active sites.

原文English
文章編號3264
期刊Nature communications
12
發行號1
DOIs
出版狀態Published - 2021 十二月

All Science Journal Classification (ASJC) codes

  • 化學 (全部)
  • 生物化學、遺傳與分子生物學 (全部)
  • 物理與天文學 (全部)

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