High Selectivity for Ethylene from Carbon Dioxide Reduction over Copper Nanocube Electrocatalysts

被引:522
作者
Roberts, F. Sloan [1 ]
Kuhl, Kendra P. [1 ]
Nilsson, Anders [1 ]
机构
[1] Stanford Univ, Dept Chem, Stanford, CA 94305 USA
关键词
carbon dioxide; electrocatalysis; electrochemical reduction; nanomaterials; ELECTROCHEMICAL REDUCTION; CO2; REDUCTION; ELECTRODES; PH;
D O I
10.1002/anie.201412214
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Nanostructured surfaces have been shown to greatly enhance the activity and selectivity of many different catalysts. Here we report a nanostructured copper surface that gives high selectivity for ethylene formation from electrocatalytic CO2 reduction. The nanostructured copper is easily formed in situ during the CO2 reduction reaction, and scanning electron microscopy (SEM) shows the surface to be dominated by cubic structures. Using online electrochemical mass spectrometry (OLEMS), the onset potentials and relative selectivity toward the volatile products (ethylene and methane) were measured for several different copper surfaces and single crystals, relating the cubic shape of the copper surface to the greatly enhanced ethylene selectivity. The ability of the cubic nanostructure to so strongly favor multicarbon product formation from CO2 reduction, and in particular ethylene over methane, is unique to this surface and is an important step toward developing a catalyst that has exclusive selectivity for multicarbon products.
引用
收藏
页码:5179 / 5182
页数:4
相关论文
共 18 条
[1]   COPPER IN SEA-WATER, POTENTIAL-PH DIAGRAMS [J].
BIANCHI, G ;
LONGHI, P .
CORROSION SCIENCE, 1973, 13 (11) :853-864
[2]   Electrochemical Reduction of CO2 using Supported Cu2O Nanoparticles [J].
Bugayong, J. ;
Griffin, G. L. .
ELECTROCHEMICAL SYNTHESIS OF FUELS 2, 2013, 58 (02) :81-89
[3]   Stable and selective electrochemical reduction of carbon dioxide to ethylene on copper mesocrystals [J].
Chen, Chung Shou ;
Handoko, Albertus D. ;
Wan, Jane Hui ;
Ma, Liang ;
Ren, Dan ;
Yeo, Boon Siang .
CATALYSIS SCIENCE & TECHNOLOGY, 2015, 5 (01) :161-168
[4]   Electrochemical reduction of carbon dioxide at various series of copper single crystal electrodes [J].
Hori, Y ;
Takahashi, I ;
Koga, O ;
Hoshi, N .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2003, 199 (1-2) :39-47
[5]  
Hori Y., 2003, Handbook of Fuel Cells: Fundamentals, Technology and Application, V2, P720
[6]   Electrochemical CO2 reduction on Cu2O-derived copper nanoparticles: controlling the catalytic selectivity of hydrocarbons [J].
Kas, Recep ;
Kortlever, Ruud ;
Milbrat, Alexander ;
Koper, Marc T. M. ;
Mul, Guido ;
Baltrusaitis, Jonas .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2014, 16 (24) :12194-12201
[7]   New insights into the electrochemical reduction of carbon dioxide on metallic copper surfaces [J].
Kuhl, Kendra P. ;
Cave, Etosha R. ;
Abram, David N. ;
Jaramillo, Thomas F. .
ENERGY & ENVIRONMENTAL SCIENCE, 2012, 5 (05) :7050-7059
[8]   Powering the planet: Chemical challenges in solar energy utilization [J].
Lewis, Nathan S. ;
Nocera, Daniel G. .
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2006, 103 (43) :15729-15735
[9]   CO2 Reduction at Low Overpotential on Cu Electrodes Resulting from the Reduction of Thick Cu2O Films [J].
Li, Christina W. ;
Kanan, Matthew W. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2012, 134 (17) :7231-7234
[10]   Scalable synthesis of hollow Cu2O nanocubes with unique optical properties via a simple hydrolysis-based approach [J].
Liu, Hui ;
Zhou, Yue ;
Kulinich, Sergei A. ;
Li, Jia-Jun ;
Han, Li-Li ;
Qiao, Shi-Zhang ;
Du, Xi-Wen .
JOURNAL OF MATERIALS CHEMISTRY A, 2013, 1 (02) :302-307