Electrocatalytic conversion of carbon dioxide to formic acid over nanosized Cu6Sn5 intermetallic compounds with a SnO2 shell layer

被引:17
作者
Gunji, Takao [1 ]
Ochiai, Hiroya [1 ]
Isawa, Yu [1 ]
Liu, Yubin [1 ]
Nomura, Fumihiro [1 ]
Miyauchi, Masahiro [2 ]
Matsumoto, Futoshi [1 ]
机构
[1] Kanagawa Univ, Dept Mat & Life Chem, Kanagawa Ku, 3-27-1 Rokkakubashi, Yokohama, Kanagawa 2218686, Japan
[2] Tokyo Inst Technol, Sch Mat & Chem Technol, Dept Mat Sci & Engn, Meguro Ku, 2-12-1 Ookayama, Tokyo 1528552, Japan
关键词
ELECTROCHEMICAL REDUCTION; CO2; REDUCTION; TIN ELECTRODES; ELECTROREDUCTION; NANOPARTICLES; SELECTIVITY; EFFICIENCY; CATALYSIS; FORMATE;
D O I
10.1039/c9cy01540j
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
A novel ordered intermetallic compound of carbon-black-supported Cu6Sn5 nanoparticles (Cu6Sn5 NP/CB) in which Cu6Sn5 has a NiAs-type structure was successfully prepared through a wet chemical method using lithium triethylborohydride as a reducing agent. The prepared ordered intermetallic compound was characterized using X-ray diffraction (XRD), transmission electron microscopy, X-ray photoelectron spectroscopy (XPS), scanning transmission electron microscopy (STEM), and X-ray absorption fine structure spectroscopy (XAFS). The XRD measurements confirm the formation of the NiAs-type ordered intermetallic Cu6Sn5. XPS and STEM-X-ray energy dispersive spectroscopy measurements allowed us to confirm the Cu6Sn5 structure. The surface of the intermetallic Cu6Sn5 was found to be covered by SnO2, indicating that a core-shell structured intermetallic compound (i.e., Cu6Sn5 core/SnO2 shell) had formed. The Cu6Sn5 NP/CB material exhibited a faradaic efficiency of 65.3% at -0.6 V for HCOO- formation via electrochemical CO2 reduction, which is superior to those of the non-intermetallic Cu NP/CB and Sn NP/CB samples. From the XAFS measurements, we determined the Sn-Sn distance in the SnO2 on the surface of the Cu6Sn5 NPs, and the key factor affecting the high selectivity was found to be the 4.9% compressive strain of the SnO2 shell layers on the Cu6Sn5 compared to that of the Sn NP/CB sample.
引用
收藏
页码:6577 / 6584
页数:8
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