Selective CO2 Electroreduction to Ethylene and Multicarbon Alcohols via Electrolyte-Driven Nanostructuring

被引：213

作者：

Gao, Dunfeng ^{[1
]}

Sinev, Ilya ^{[1
,2
]}

Scholten, Fabian ^{[1
,2
]}

Aran-Ais, Rosa M. ^{[1
]}

Divins, Nuria J. ^{[1
,2
]}

Kvashnina, Kristina ^{[3
,4
]}

Timoshenko, Janis ^{[1
]}

Roldan Cuenya, Beatriz ^{[1
]}

机构：

[1] Max Planck Gesell, Dept Interface Sci, Fritz Haber Inst, D-14195 Berlin, Germany

[2] Ruhr Univ Bochum, Dept Phys, D-44780 Bochum, Germany

[3] ESRF European Synchrotron, Rossendorf Beamline, CS40220, F-38043 Grenoble 9, France

[4] Helmholtz Zentrum Dresden Rossendorf, Inst Resource Ecol, POB 510119, D-01314 Dresden, Germany

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2019年 / 58卷 / 47期

基金：

欧洲研究理事会;

关键词：

adsorbed halides; CO2; electroreduction; copper(I); electrolyte-driven nanostructuring; multicarbon products; CARBON-DIOXIDE; ELECTROCHEMICAL REDUCTION; SPECTROSCOPIC OBSERVATION; COPPER; CATALYSTS; HYDROCARBONS; OXIDATION; DESIGN;

D O I：

10.1002/anie.201910155

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Production of multicarbon products (C2+) from CO2 electroreduction reaction (CO2RR) is highly desirable for storing renewable energy and reducing carbon emission. The electrochemical synthesis of CO2RR catalysts that are highly selective for C2+ products via electrolyte-driven nanostructuring is presented. Nanostructured Cu catalysts synthesized in the presence of specific anions selectively convert CO2 into ethylene and multicarbon alcohols in aqueous 0.1m KHCO3 solution, with the iodine-modified catalyst displaying the highest Faradaic efficiency of 80% and a partial geometric current density of ca. 31.2 mA cm(-2) for C2+ products at -0.9V vs. RHE. Operando X-ray absorption spectroscopy and quasi insitu X-ray photoelectron spectroscopy measurements revealed that the high C2+ selectivity of these nanostructured Cu catalysts can be attributed to the highly roughened surface morphology induced by the synthesis, presence of subsurface oxygen and Cu+ species, and the adsorbed halides.

引用

页码：17047 / 17053

页数：7

共 49 条

[1]

[Anonymous], 2015, ANGEW CHEM, DOI DOI 10.1002/ANGE.201412214

[2] Structure- and Electrolyte-Sensitivity in CO2 Electroreduction [J].

Aran-Ais, Rosa M. ;

Gao, Dunfeng ;

Roldan Cuenya, Beatriz .

ACCOUNTS OF CHEMICAL RESEARCH, 2018, 51 (11) :2906-2917

[3] Electrochemical CO Reduction: A Property of the Electrochemical Interface [J].

Bagger, Alexander ;

Arnarson, Logi ;

Hansen, Martin H. ;

Spohr, Eckhard ;

Rossmeisl, Jan .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2019, 141 (04) :1506-1514

[4]

Cavalca F., 2017, J PHYS CHEM C, V121, P25010

[5] Enhanced Stability and CO/Formate Selectivity of Plasma-Treated SnOx/AgOx Catalysts during CO2 Electroreduction [J].

Choi, Yong-Wook ;

Scholten, Fabian ;

Sinev, Ilya ;

Roldan Cuenya, Beatriz .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2019, 141 (13) :5261-5266

[6] Catalyst electro-redeposition controls morphology and oxidation state for selective carbon dioxide reduction [J].

De Luna, Phil ;

Quintero-Bermudez, Rafael ;

Cao-Thang Dinh ;

Ross, Michael B. ;

Bushuyev, Oleksandr S. ;

Todorovic, Petar ;

Regier, Tom ;

Kelley, Shana O. ;

Yang, Peidong ;

Sargent, Edward H. .

NATURE CATALYSIS, 2018, 1 (02) :103-110

[7] On the Role of Sulfur for the Selective Electrochemical Reduction of CO2 to Formate on CuSx Catalysts [J].

Deng, Yilin ;

Huang, Yun ;

Ren, Dan ;

Handoko, Albertus D. ;

Seh, Zhi Wei ;

Hirunsit, Pussana ;

Yeo, Boon Siang .

ACS APPLIED MATERIALS & INTERFACES, 2018, 10 (34) :28572-28581

[8] Morphology Matters: Tuning the Product Distribution of CO2 Electroreduction on Oxide-Derived Cu Foam Catalysts [J].

Dutta, Abhijit ;

Rahaman, Motiar ;

Luedi, Nicola C. ;

Broekmann, Peter .

ACS CATALYSIS, 2016, 6 (06) :3804-3814

[9] Subsurface Oxygen in Oxide-Derived Copper Electrocatalysts for Carbon Dioxide Reduction [J].

Eilert, Andre ;

Cavalca, Filippo ;

Roberts, F. Sloan ;

Osterwalder, Juerg ;

Liu, Chang ;

Favaro, Marco ;

Crumlin, Ethan J. ;

Ogasawara, Hirohito ;

Friebel, Daniel ;

Pettersson, Lars G. M. ;

Nilsson, Anders .

JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 2017, 8 (01) :285-290

[10] Subsurface oxide plays a critical role in CO2 activation by Cu(111) surfaces to form chemisorbed CO2, the first step in reduction of CO2 [J].

Favaro, Marco ;

Xiao, Hai ;

Cheng, Tao ;

Goddard, William A., III ;

Yano, Junko ;

Crumlin, Ethan J. .

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2017, 114 (26) :6706-6711

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