Jinfeng Jia, Jiayi Chen, Ioannis Katsounaros, Emiel de Smit, Saifudin M Abubakar, Shuo Chen, Lei Wang, Yanwei Lum
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引用次数: 0
摘要
调节催化剂和溶剂之间的相互作用为调整电化学CO2还原（CO2R）的选择性提供了一种有前途的策略。本文研究了以Pb为原料，通过CO2R法制备草酸盐（C2O42-）。然后研究了铅箔在乙腈（ACN）、二甲基甲酰胺（DMF）、二甲基亚砜（DMSO）和碳酸丙烯（PC）等非质子电解质中的CO2R性能。我们发现溶剂极性和氢键给体能力显著影响反应选择性。值得注意的是，DMF在15 mA cm-2下表现出88%的草酸法拉第效率（FE），这是由于增强了反应中间体的稳定性和降低了析氢反应（HER）活性。最后，建立了一种基于滴定法的草酸盐定量分析方法，该方法适用于各种非质子电解质，并且提供了一种简单快速的方法，并通过高效液相色谱（HPLC）进行了验证。
Investigating the electrochemical reduction of CO2 to oxalate in aprotic solvents with Pb.
Modulating the interaction between the catalyst and solvent offers a promising strategy to tune selectivity in electrochemical CO2 reduction (CO2R). In this work, we investigated the production of oxalate (C2O42-) through CO2R using Pb. Then we studied the CO2R performance of Pb foil in various aprotic electrolytes, including acetonitrile (ACN), dimethylformamide (DMF), dimethyl sulfoxide (DMSO) and propylene carbonate (PC). We found that solvent polarity and hydrogen bond donor ability significantly affect reaction selectivity. Notably, DMF exhibited an oxalate Faradaic efficiency (FE) of 88% at 15 mA cm-2, attributed to enhanced stabilization of reaction intermediates and reduced hydrogen evolution reaction (HER) activity. Finally, a titration-based analytical method for oxalate quantification was developed, suitable for various aprotic electrolytes and offering a simple and rapid approach, which we validated using high-performance liquid chromatography (HPLC).
期刊介绍：
ChemPhysChem is one of the leading chemistry/physics interdisciplinary journals (ISI Impact Factor 2018: 3.077) for physical chemistry and chemical physics. It is published on behalf of Chemistry Europe, an association of 16 European chemical societies.
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