Acetaldehyde as an Intermediate in the Electroreduction of Carbon Monoxide to Ethanol on Oxide-Derived Copper

被引：186

作者：

Bertheussen, Erlend ^{[1
]}

Verdaguer-Casadevall, Arnau ^{[1
]}

Ravasio, Davide ^{[2
]}

Montoya, Joseph H. ^{[3
]}

Trimarco, Daniel B. ^{[1
]}

Roy, Claudie ^{[1
]}

Meier, Sebastian ^{[4
]}

Wendland, Juergen ^{[2
]}

Norskov, Jens K. ^{[5
]}

Stephens, Ifan E. L. ^{[1
,6
]}

Chorkendorff, Ib ^{[1
]}

机构：

[1] Tech Univ Denmark, Dept Phys, DK-2800 Lyngby, Denmark

[2] Carlsberg Lab, Gamle Carlsberg Vej 4, DK-1799 Copenhagen V, Denmark

[3] Stanford Univ, Dept Chem Engn, SUNCAT Ctr Catalysis & Interface Sci, 443 Via Ortega, Stanford, CA 94305 USA

[4] Tech Univ Denmark, Dept Chem, DK-2800 Lyngby, Denmark

[5] SLAC Natl Accelerator Lab, SUNCAT Ctr Catalysis & Interface Sci, 2675 Sand Hill Rd, Menlo Pk, CA 94025 USA

[6] MIT, Dept Mech Engn, Cambridge, MA 02319 USA

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2016年 / 55卷 / 04期

关键词：

analytical chemistry; catalysis; electrochemistry; energy conversion; materials science; ELECTROCHEMICAL REDUCTION; CO2; REDUCTION; DIOXIDE REDUCTION; IN-SITU; INSIGHTS;

D O I：

10.1002/anie.201508851

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Oxide-derived copper (OD-Cu) electrodes exhibit unprecedented CO reduction performance towards liquid fuels, producing ethanol and acetate with >50% Faradaic efficiency at 0.3 V (vs. RHE). By using static headspace-gas chromatography for liquid phase analysis, we identify acetaldehyde as a minor product and key intermediate in the electroreduction of CO to ethanol on OD-Cu electrodes. Acetaldehyde is produced with a Faradaic efficiency of approximate to 5% at -0.33 V (vs. RHE). We show that acetaldehyde forms at low steady-state concentrations, and that free acetaldehyde is difficult to detect in alkaline solutions using NMR spectroscopy, requiring alternative methods for detection and quantification. Our results represent an important step towards understanding the CO reduction mechanism on OD-Cu electrodes.

引用

页码：1450 / 1454

页数：5

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