Electrocatalytic Reduction of CO2 to Acetic Acid by a Molecular Manganese Corrole Complex

被引：131

作者：

De, Ratnadip ^{[1
]}

Gonglach, Sabrina ^{[2
]}

Paul, Shounik ^{[1
]}

Haas, Michael ^{[2
]}

Sreejith, S. S. ^{[1
]}

Gerschel, Philipp ^{[3
]}

Apfel, Ulf-Peter ^{[3
,4
]}

Vuong, Thanh Huyen ^{[5
]}

Rabeah, Jabor ^{[5
]}

Roy, Soumyajit ^{[1
]}

Schoefberger, Wolfgang ^{[2
]}

机构：

[1] Indian Inst Sci Educ & Res, Ecofriendly Appl Mat Lab EFAML, Ctr Mat Sci, Dept Chem Sci, Mohanpur Campus, Kolkata 741246, W Bengal, India

[2] Johannes Kepler Univ Linz, Inst Organ Chem, Altenberger Str 69, Linz 4040, Austria

[3] Ruhr Univ Bochum, Inorgan Chem 1, Univ Str 150, Bochum 44801, Germany

[4] Fraunhofer UMSICHT, Osterfelder Str 3, Oberhausen 46047, Germany

[5] Leibniz Inst Katalyse eV, Albert Einstein Str 29a, Rostock 18059, Germany

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2020年 / 59卷 / 26期

基金：

奥地利科学基金会;

关键词：

acetic acid; carbon dioxide; electrocatalysis; manganese corrole; reduction; ELECTROCHEMICAL REDUCTION; REDOX POTENTIALS; CARBON-DIOXIDE; CATALYST; SELECTIVITY; ACETATE; SOLVENT;

D O I：

10.1002/anie.202000601

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The controlled electrochemical reduction of carbon dioxide to value added chemicals is an important strategy in terms of renewable energy technologies. Therefore, the development of efficient and stable catalysts in an aqueous environment is of great importance. In this context, we focused on synthesizing and studying a molecular Mn-III-corrole complex, which is modified on the three meso-positions with polyethylene glycol moieties for direct and selective production of acetic acid from CO2. Electrochemical reduction of Mn-III leads to an electroactive Mn-II species, which binds CO2 and stabilizes the reduced intermediates. This catalyst allows to electrochemically reduce CO2 to acetic acid in a moderate acidic aqueous medium (pH 6) with a selectivity of 63 % and a turn over frequency (TOF) of 8.25 h(-1), when immobilized on a carbon paper (CP) electrode. In terms of high selectivity towards acetate, we propose the formation and reduction of an oxalate type intermediate, stabilized at the Mn-III-corrole center.

引用

页码：10527 / 10534

页数：8

共 31 条

[1]

[Anonymous], 2019, Global Energy CO2 Status Report 2019.

[2] Catalysis for the Valorization of Exhaust Carbon: from CO2 to Chemicals, Materials, and Fuels. Technological Use of CO2 [J].