The pH and Potential Dependence of Pb‐Catalyzed Electrochemical CO 2 Reduction to Methyl Formate in a Dual Methanol/Water Electrolyte
The pH and Potential Dependence of Pb‐Catalyzed Electrochemical CO 2 Reduction to Methyl Formate in a Dual Methanol/Water Electrolyte
复制标题
双甲醇/水电解质中 Pb 催化 CO 2 电化学还原成甲酸甲酯的 pH 和电位依赖性
DOI：
10.1002/cssc.202102289
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发表时间：
2022
期刊：
影响因子：
8.4
通讯作者：
Spurgeon, Joshua M.
中科院分区：
文献类型：
--
作者：
Hofsommer, Dillon T.;Liang, Ying;Uttarwar, Sandesh S.;Gautam, Manu;Pishgar, Sahar;Gulati, Saumya;Grapperhaus, Craig A.;Spurgeon, Joshua M.
通过电化学还原将废二氧化碳转化为增值化学品是一项很有前途的技术，可以减缓气候变化，同时提供经济机会。使用非水溶剂，如甲醇，可以获得更高的二氧化碳利用率和新的产品。在这项工作中，研究了在酸性甲醇阴极液中，二氧化碳在铅工作电极上的电化学还原，同时使用单独的水阳极液来促进可持续的水氧化半反应。甲酸甲酯(一种在甲醇中还原二氧化碳的独特产物)、甲酸和甲酸盐之间的选择性严重依赖于阴极液的pH，较高的pH条件导致甲酸盐，而低pH条件有利于甲酸甲酯。还研究了产物在酸性阴极液中分布的电势依赖性，在 2.0−Vvs.Ag/ 时，甲酸甲酯的法拉第效率高达75%。
The conversion of waste CO2to value‐added chemicals through electrochemical reduction is a promising technology for mitigating climate change while simultaneously providing economic opportunities. The use of non‐aqueous solvents like methanol allows for higher CO2availability and novel products. In this work, the electrochemistry of CO2reduction in acidic methanol catholyte at a Pb working electrode was investigated while using a separate aqueous anolyte to promote a sustainable water oxidation half‐reaction. The selectivity among methyl formate (a product unique to reduction of CO2in methanol), formic acid, and formate was critically dependent on the catholyte pH, with higher pH conditions leading to formate and low pH favoring methyl formate. The potential dependence of the product distribution in acidic catholyte was also investigated, with a faradaic efficiency for methyl formate as high as 75 % measured at −2.0 V vs. Ag/AgCl.