期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 124, 期 43, 页码 23764-23772出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.0c07556
关键词
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资金
- Genie des Procedes PhD Program of Sorbonne Universite
- Onassis foundation [F ZO 012-1/2018-2019]
The structure effect on the role of different ionic liquids (ILs) as a simultaneous supporting electrolyte and cocatalyst for CO2 electroreduction in the presence of a model molecular catalyst [Re(bpy)(CO)(3)Cl] has not been addressed yet. In particular, we varied the nature of the cation, anion, and cation alkyl chain by a choice of five different ILs, including imidazolium and pyrrolidinium cations, and we compared their results to benchmark the supporting electrolyte. We report an overpotential diminution of 0.33 V for CO2 to CO conversion in the presence of ILs under CO2 catalytic conditions. We prove the IL cation-dependent overpotential diminution due to the electrostatic stabilization of the negatively charged active form of the catalyst, with the pi-pi stacking interaction provided by imidazolium cations responsible for their outstanding performance. Finally, a mechanistic explanation is provided to justify a weaker IL cocatalytic effect when CO2 electroreduction takes place in the presence of a proton source.
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