Ponsard Louise, Nicolas Emmanuel, Tran Ngoc Huan, Lamaison Sarah, Wakerley David, Cantat Thibault, Fontecave Marc
Université Paris-Saclay, CEA, CNRS, NIMBE, 91191, Gif-sur-Yvette, France.
Laboratoire de Chimie des Processus Biologiques, CNRS UMR 8229, Collège de France, Sorbonne Université, 11 Place Marcelin Berthelot, 75231, Paris Cedex 05, France.
ChemSusChem. 2021 May 20;14(10):2198-2204. doi: 10.1002/cssc.202100459. Epub 2021 Mar 25.
Carbonylation reactions that generate high-value chemical feedstocks are integral to the formation of many industrially significant compounds. However, these processes require the use of CO, which is invariably derived from fossil-fuel-reforming reactions. CO may also be generated through the electroreduction of CO , but the coupling of these two processes is yet to be considered. Merging electrocatalytic reduction of CO to CO with thermocatalytic use of CO would expand the range of the chemicals produced from CO . This work describes the development of a system coupling a high-pressure CO electrolytic cell containing a bimetallic ZnAg catalyst at the cathode for production of CO with a reactor with a Faradaic efficiency of >90 % where high pressure CO is used for carbonylating propylene oxide into β-butyrolactone by thermal catalysis, the latter step having a reaction yield above 80 %. Although the production of monomers and polymers from CO is currently limited to organic carbonates, this strategy opens up the access to lactones from CO , for the formation of polyesters.
生成高价值化学原料的羰基化反应是许多具有工业重要性的化合物形成过程中不可或缺的一部分。然而，这些过程需要使用一氧化碳，而一氧化碳总是来源于化石燃料重整反应。一氧化碳也可以通过一氧化碳的电还原生成，但这两个过程的耦合尚未得到考虑。将一氧化碳的电催化还原与一氧化碳的热催化利用相结合，将扩大由一氧化碳生产的化学品范围。这项工作描述了一种系统的开发，该系统将一个高压一氧化碳电解池与一个反应器耦合，该电解池在阴极含有双金属锌银催化剂以生产一氧化碳，法拉第效率>90%，在该反应器中，高压一氧化碳通过热催化用于将环氧丙烷羰基化为β-丁内酯，后一步反应产率高于80%。尽管目前由一氧化碳生产单体和聚合物仅限于有机碳酸盐，但这种策略为从一氧化碳获取内酯以形成聚酯开辟了道路。
