Electrokinetic and in situ spectroscopic investigations of CO electrochemical reduction on copper
| Autor: | Qi Lu, Bingjun Xu, Xiaoxia Chang, Haochen Zhang, Arnav S. Malkani, Mu Jeng Cheng, Jing Li |
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| Rok vydání: | 2021 |
| Předmět: |
Tafel equation
Reaction mechanism Multidisciplinary Order of reaction Chemistry Science Inorganic chemistry General Physics and Astronomy 02 engineering and technology General Chemistry Electrolyte 010402 general chemistry 021001 nanoscience & nanotechnology Electrochemistry 01 natural sciences Redox General Biochemistry Genetics and Molecular Biology Article 0104 chemical sciences Catalysis Proton-coupled electron transfer 0210 nano-technology Electrocatalysis |
| Zdroj: | Nature Communications Nature Communications, Vol 12, Iss 1, Pp 1-11 (2021) |
| ISSN: | 2041-1723 |
| Popis: | 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 11) alkaline electrolytes, respectively. Further, CH4 and C2+ products are likely formed on distinct types of active sites. Electrokinetic results are key to understanding the mechanisms in electrochemical CO reduction reaction. Here, the authors determine mass transport free kinetics using a gas-diffusion electrode and identified dependence of copper surface speciation on the electrolyte pH using in situ surface enhanced spectroscopies. |
| Databáze: | OpenAIRE |
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