Optimising the electrochemical reduction of CO 2 to oxalic acid in propylene carbonate
Optimising the electrochemical reduction of CO 2 to oxalic acid in propylene carbonate
复制标题
优化碳酸亚丙酯中CO 2 电化学还原为草酸的过程
DOI：
10.1039/d3se00652b
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发表时间：
2023
影响因子：
5.6
通讯作者：
Sale H
中科院分区：
文献类型：
--
作者：
Sale H
二氧化碳（从大气中捕获或通过其他途径获得）是生产许多有价值的化学品和燃料的有用和广泛可用的组成部分。用于二氧化碳还原的电化学方法在可扩展性、直接耦合到可再生电源的前景以及在不共同产生有害副产物的情况下还原二氧化碳的能力方面提供了优势。在二氧化碳电还原的各种可能产物中，草酸盐/草酸是特别有吸引力的目标，因为其广泛用于许多化学和制药过程。本文报道了在碳酸丙烯酯溶剂体系中，加入苯甲腈催化二氧化碳电还原为草酸盐/草酸的研究结果。我们的研究结果表明，使用苯甲腈作为均相电催化剂提高了草酸盐/草酸生产的法拉第和反应产率，以及草酸盐/草酸形成的面积归一化速率，在电压为-2.7 V vs. SCE（-2.46 V vs. SHE）时，形成速率达到1.65 ± 0.35 mM cm−2 h−1（1 h平均值）的新记录。这些指标反过来表明，通过草酸盐将二氧化碳电化学还原为C2+产物可能是进一步开发关键化学原料可持续生产的有希望的途径。
Carbon dioxide (captured from the atmosphere or obtained by other routes) constitutes a useful and widely available building block for producing numerous valuable chemicals and fuels. Electrochemical methods for carbon dioxide reduction offer advantages in terms of scalability, the prospect of coupling directly to renewable power sources and the ability to reduce carbon dioxide without the co-production of harmful by-products. Of the various possible products of carbon dioxide electroreduction, oxalate/oxalic acid is an especially attractive target because of its wide use in many chemical and pharmaceutical processes. Herein, we report the results of a study on carbon dioxide electroreduction to oxalate/oxalic acid in a propylene carbonate solvent system, catalysed by the addition of benzonitrile. Our results show that the use of benzonitrile as a homogeneous electrocatalyst improves the faradaic and reaction yields of oxalate/oxalic acid production, as well as the area-normalised rate of formation of oxalate/oxalic acid, giving a new record rate of formation of 1.65 ± 0.35 mM cm−2 h−1 (averaged over 1 h) at a voltage of –2.7 V vs. SCE (–2.46 V vs. SHE). Such metrics in turn suggest that the electrochemical reduction of carbon dioxide to C2+ products via oxalate could be a promising avenue for further development for the sustainable production of key chemical feedstocks.