Electrochemically Generated Copper Carbonyl for Selective Dimethyl Carbonate Synthesis

被引:18
|
作者
Davies, Bethan J. V. [1 ]
Saric, Manuel [1 ,2 ]
Figueiredo, Marta C. [1 ,5 ]
Schjodt, Niels C. [3 ]
Dahl, Soren [3 ]
Moses, Poul Georg [3 ]
Escudero-Escribano, Maria [1 ]
Arenz, Matthias [1 ,4 ]
Rossmeisl, Jan [1 ]
机构
[1] Univ Copenhagen, Dept Chem, Nanosci Ctr, Univ Pk 5, DK-2100 Copenhagen, Denmark
[2] Tech Univ Denmark, Dept Phys, Ctr Atom Scale Mat Design CAMd, Fys Vej Bldg 307, DK-2800 Lyngby, Denmark
[3] Haldor Topsoe A S, Nymollevej 55, DK-2800 Lyngby, Denmark
[4] Univ Bern, Dept Chem & Biochem, Freiestr 3, CH-3012 Bern, Switzerland
[5] Avantium, Zekeringstr 29, NL-1014 BV Amsterdam, Netherlands
来源
ACS CATALYSIS | 2019年 / 9卷 / 02期
关键词
copper; dimethyl carbonate; electrosynthesis; spectroelectrochemistry; methanol; ELECTROLYTIC CARBONYLATION; INFRARED-SPECTROSCOPY; METHANOL; ANODE; CO; ELECTROOXIDATION; REDUCTION; CHEMISTRY; DMC;
D O I
10.1021/acscatal.8b03682
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Development of electrochemical synthesis routes for high-value chemicals could pave the way for a sustainable chemical industry based on electricity. Herein, the electrochemical synthesis of the industrially relevant and environmentally benign reagent, dimethyl carbonate (DMC), is investigated. By utilizing a combination of electrochemical techniques, in situ infrared spectroscopy, and headspace-gas chromatography-mass spectrometry we show production and spectroelectrochemical evidence for the synthesis of DMC via an electrochemically generated copper carbonyl species. The formation of the copper carbonyl has close to 100% current efficiency, in the applied potential range of 0.1-0.4 V vs SCE. Subsequent formation of DMC occurs with a slow reaction time on the order of 30-40 days. Relative to potential coproducts, the reaction is highly selective for DMC. Optimization of the reaction may lead to a viable method of DMC production.
引用
收藏
页码:859 / 866
页数:15
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