Mesoporous palladium-copper bimetallic electrodes for selective electrocatalytic reduction of aqueous CO2 to CO

被引:123
作者
Li, Mu [1 ,2 ,3 ]
Wang, Junjie [1 ,2 ]
Li, Peng [1 ,2 ]
Chang, Kun [1 ,2 ]
Li, Cuiling [1 ,2 ]
Wang, Tao [1 ,2 ]
Jiang, Bo [1 ,2 ]
Zhang, Huabin [1 ,2 ]
Liu, Huimin [1 ,2 ]
Yamauchi, Yusuke [1 ,2 ,4 ]
Umezawa, Naoto [1 ,2 ,3 ,4 ]
Ye, Jinhua [1 ,2 ,3 ,4 ,5 ]
机构
[1] Natl Inst Mat Sci, Environm Remediat Mat Unit, 1-1 Namiki, Tsukuba, Ibaraki 3050044, Japan
[2] Natl Inst Mat Sci, Int Ctr Mat Nanoarchitecton MANA, 1-1 Namiki, Tsukuba, Ibaraki 3050044, Japan
[3] Hokkaido Univ, Grad Sch Chem Sci & Engn, Sapporo, Hokkaido 0600814, Japan
[4] Tianjin Univ, TU NIMS Joint Res Ctr, Sch Mat Sci & Engn, 92 Weijin Rd, Tianjin 300072, Peoples R China
[5] Collaborat Innovat Ctr Chem Sci & Engn Tianjin, Tianjin 300072, Peoples R China
基金
奥地利科学基金会;
关键词
CARBON-DIOXIDE; ELECTROCHEMICAL REDUCTION; CONVERSION; PD; ELECTROREDUCTION; SURFACE;
D O I
10.1039/c6ta00487c
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
Finding a highly efficient, selective and economic approach for electrochemical reduction of aqueous carbon dioxide is a great challenge in realizing an artificial system for a sustainable carbon cycle. Novel mesoporous palladium-copper bimetallic electrocatalysts with superior activity and high faradaic efficiencies (FEs) are reported for the first time. The mesoporous nanostructure provides a roughened surface which is abundant in active sites and promotes selective conversion of CO2 to CO. First-principles calculations exhibit that Pd atoms on the catalyst surface serve as reactive centers and highly selective CO formation is attributed to the geometric and electronic effects within the palladium-copper bimetallic alloys. The CO2 and COOH* intermediate adsorption ability and the CO desorption ability on Pd atoms are effectively enhanced in the presence of Cu. Our results provide wide ranging implications for further improving the design and preparation of CO2 reduction electrocatalysts.
引用
收藏
页码:4776 / 4782
页数:7
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