Electrodeposited Zn Dendrites with Enhanced CO Selectivity for Electrocatalytic CO2 Reduction

被引:398
作者
Rosen, Jonathan [1 ]
Hutchings, Gregory S. [1 ]
Lu, Qi [1 ]
Forest, Robert V. [1 ]
Moore, Alex [1 ]
Jiao, Feng [1 ]
机构
[1] Univ Delaware, Dept Biomol & Chem Engn, Ctr Catalyt Sci & Technol, Newark, DE 19716 USA
来源
ACS CATALYSIS | 2015年 / 5卷 / 08期
基金
美国国家科学基金会;
关键词
electrocatalysis; CO2; reduction; Zn; electrodeposition; X-ray absorption spectroscopy; ELECTROCHEMICAL REDUCTION; CARBON-DIOXIDE; METAL-ELECTRODES; ZINC; CONVERSION; CATALYSTS;
D O I
10.1021/acscatal.5b00922
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Electrochemical CO2 reduction is a key reaction for CO2 conversion to valuable fuels and chemicals. Because of the high stability of the CO2 molecule, a catalyst is typically required to minimize the energy input and improve reaction rates needed for device level commercialization. In this paper, we report a nanostructured Zn dendrite catalyst that is able to electrochemically reduce CO2 to CO in an aqueous bicarbonate electrolyte with greatly enhanced properties. The catalytic activity is over an order of magnitude higher than that of bulk Zn counterparts, with a CO faradaic efficiency around 3-fold higher. The stability of the Zn electrode under realistic CO2 electrolysis conditions was explored using scanning electron microscopy and in situ/operando X-ray absorption spectroscopy techniques. The results clearly demonstrate that nanostructured and bulk Zn catalysts are structurally stable at potentials more negative than -0.7 V versus RHE, whereas severe chemical oxidation occurs at more positive potentials.
引用
收藏
页码:4586 / 4591
页数:6
相关论文
共 25 条
[1]   ELECTROCHEMICAL REDUCTION OF CARBON-DIOXIDE ON VARIOUS METAL-ELECTRODES IN LOW-TEMPERATURE AQUEOUS KHCO3 MEDIA [J].
AZUMA, M ;
HASHIMOTO, K ;
HIRAMOTO, M ;
WATANABE, M ;
SAKATA, T .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 1990, 137 (06) :1772-1778
[2]   Aqueous CO2 Reduction at Very Low Overpotential on Oxide-Derived Au Nanoparticles [J].
Chen, Yihong ;
Li, Christina W. ;
Kanan, Matthew W. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2012, 134 (49) :19969-19972
[3]   Electrodeposition of preferentially oriented zinc for flow-assisted alkaline batteries [J].
Desai, Divyaraj ;
Wei, Xia ;
Steingart, Daniel A. ;
Banerjee, Sanjoy .
JOURNAL OF POWER SOURCES, 2014, 256 :145-152
[4]   ELECTROCATALYTIC PROCESS OF CO SELECTIVITY IN ELECTROCHEMICAL REDUCTION OF CO2 AT METAL-ELECTRODES IN AQUEOUS-MEDIA [J].
HORI, Y ;
WAKEBE, H ;
TSUKAMOTO, T ;
KOGA, O .
ELECTROCHIMICA ACTA, 1994, 39 (11-12) :1833-1839
[5]  
Hori Y, 2008, MOD ASP ELECTROCHEM, P89
[6]   PRODUCTION OF CO AND CH4 IN ELECTROCHEMICAL REDUCTION OF CO2 AT METAL-ELECTRODES IN AQUEOUS HYDROGENCARBONATE SOLUTION [J].
HORI, Y ;
KIKUCHI, K ;
SUZUKI, S .
CHEMISTRY LETTERS, 1985, (11) :1695-1698
[7]   Zinc ion effect on the electrochemical reduction of carbon dioxide at zinc electrode in aqueous solutions [J].
Ikeda, S ;
Hattori, A ;
Ito, K ;
Noda, H .
ELECTROCHEMISTRY, 1999, 67 (01) :27-33
[8]   Electrochemical reduction behavior of carbon dioxide on sintered zinc oxide electrode in aqueous solution [J].
Ikeda, S ;
Hattori, A ;
Maeda, M ;
Ito, K ;
Noda, H .
ELECTROCHEMISTRY, 2000, 68 (04) :257-261
[9]   Synergistic geometric and electronic effects for electrochemical reduction of carbon dioxide using gold-copper bimetallic nanoparticles [J].
Kim, Dohyung ;
Resasco, Joaquin ;
Yu, Yi ;
Asiri, Abdullah Mohamed ;
Yang, Peidong .
NATURE COMMUNICATIONS, 2014, 5
[10]   Electrocatalytic Conversion of Carbon Dioxide to Methane and Methanol on Transition Metal Surfaces [J].
Kuhl, Kendra P. ;
Hatsukade, Toru ;
Cave, Etosha R. ;
Abram, David N. ;
Kibsgaard, Jakob ;
Jaramillo, Thomas F. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2014, 136 (40) :14107-14113