甲醇
催化作用
格式化
一氧化碳
二氧化碳电化学还原
化学
钴
无机化学
法拉第效率
水溶液
电化学
甲醛
材料科学
有机化学
电极
物理化学
作者
Etienne Boutin,Min Wang,Joseph Lin,Matthieu Mesnage,Daniela Mendoza,Benedikt Lassalle‐Kaiser,Christopher Hahn,Thomas F. Jaramillo,Marc Robert
标识
DOI:10.1002/anie.201909257
摘要
Conversion of CO2 into valuable molecules is a field of intensive investigation with the aim of developing scalable technologies for making fuels using renewable energy sources. While electrochemical reduction into CO and formate are approaching industrial maturity, a current challenge is obtaining more reduced products like methanol. However, literature on the matter is scarce, and even more for the use of molecular catalysts. Here, we demonstrate that cobalt phthalocyanine, a well-known catalyst for the electrochemical conversion of CO2 to CO, can also catalyze the reaction from CO2 or CO to methanol in aqueous electrolytes at ambient conditions of temperature and pressure. The studies identify formaldehyde as a key intermediate and an unexpected pH effect on selectivity. This paves the way for establishing a sequential process where CO2 is first converted to CO which is subsequently used as a reactant to produce methanol. Under ideal conditions, the reaction shows a global Faradaic efficiency of 19.5 % and chemical selectivity of 7.5 %.
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