Electrochemically Generated Copper Carbonyl for Selective Dimethyl Carbonate Synthesis

Bethan  Davies; Manuel Saric; Marta Figueiredo; Niels Schjødt; Søren Dahl; Poul Moses; Maria Escudero Escribano; Matthias Arenz; Jan Rossmeisl

doi:10.1021/acscatal.8b03682

Electrochemically Generated Copper Carbonyl for Selective Dimethyl Carbonate Synthesis

Bethan Davies, Manuel Saric, Marta Figueiredo, Niels Schjødt, Søren Dahl, Poul Moses, Maria Escudero Escribano^*, Matthias Arenz, Jan Rossmeisl

^*Corresponding author af dette arbejde

Kemisk Institut

7 Citationer (Scopus)

Abstract

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.

Originalsprog	Engelsk
Tidsskrift	ACS Catalysis
Vol/bind	9
Udgave nummer	2
Sider (fra-til)	859-866
Antal sider	8
ISSN	2155-5435
DOI	https://doi.org/10.1021/acscatal.8b03682
Status	Udgivet - 1 feb. 2019

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10.1021/acscatal.8b03682

Citationsformater

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title = "Electrochemically Generated Copper Carbonyl for Selective Dimethyl Carbonate Synthesis",

abstract = "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.",

author = "Bethan Davies and Manuel Saric and Marta Figueiredo and Niels Schj{\o}dt and S{\o}ren Dahl and Poul Moses and {Escudero Escribano}, Maria and Matthias Arenz and Jan Rossmeisl",

year = "2019",

month = feb,

day = "1",

doi = "10.1021/acscatal.8b03682",

language = "English",

volume = "9",

pages = "859--866",

journal = "ACS Catalysis",

issn = "2155-5435",

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TY - JOUR

T1 - Electrochemically Generated Copper Carbonyl for Selective Dimethyl Carbonate Synthesis

AU - Davies, Bethan

AU - Saric, Manuel

AU - Figueiredo, Marta

AU - Schjødt, Niels

AU - Dahl, Søren

AU - Moses, Poul

AU - Escudero Escribano, Maria

AU - Arenz, Matthias

AU - Rossmeisl, Jan

PY - 2019/2/1

Y1 - 2019/2/1

N2 - 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.

AB - 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.

U2 - 10.1021/acscatal.8b03682

DO - 10.1021/acscatal.8b03682

M3 - Journal article

SN - 2155-5435

VL - 9

SP - 859

EP - 866

JO - ACS Catalysis

JF - ACS Catalysis

IS - 2

ER -

Electrochemically Generated Copper Carbonyl for Selective Dimethyl Carbonate Synthesis

Abstract

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