文献类型：期刊文献

英文题名：Homogeneously dispersed multimetal oxygen-evolving catalysts

作者：Zhang, Bo[1,2];Zheng, Xueli[1,3];Voznyy, Oleksandr[1];Comin, Riccardo[1];Bajdich, Michal[4,5];Garcia-Melchor, Max[4,5];Han, Lili[6];Xu, Jixian[1];Liu, Min[1];Zheng, Lirong[7];de Arquer, F. Pelayo Garcia[1];Dinh, Cao Thang[1];Fan, Fengjia[1];Yuan, Mingjian[1];Yassitepe, Emre[1];Chen, Ning[8];Regier, Tom[8];Liu, Pengfei[9];Li, Yuhang[9];De Luna, Phil[1];Janmohamed, Alyf[1];Xin, Huolin L.[6];Yang, Huagui[9];Vojvodic, Aleksandra[4,5];Sargent, Edward H.[1]

机构：[1]Univ Toronto, Dept Elect & Comp Engn, 35 St George St, Toronto, ON M5S 1A4, Canada;[2]E China Univ Sci & Technol, Dept Phys, 130 Meilong Rd, Shanghai 200237, Peoples R China;[3]Tianjin Univ, Sch Mat Sci & Engn, Tianjin Key Lab Composite & Funct Mat, Tianjin 300072, Peoples R China;[4]Stanford Univ, Dept Chem Engn, SUNCAT Ctr Interface Sci & Catalysis, Stanford, CA 94305 USA;[5]SLAC Natl Accelerator Lab, 2575 Sand Hill Rd, Menlo Pk, CA 94025 USA;[6]Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA;[7]Chinese Acad Sci, Beijing Synchrotron Radiat Facil, Inst High Energy Phys, Beijing 100049, Peoples R China;[8]Canadian Light Source CLS, 44 Innovation Blvd, Saskatoon, SK S7N 2V3, Canada;[9]E China Univ Sci & Technol, Sch Mat Sci & Engn, Key Lab Ultrafine Mat, Minist Educ, 130 Meilong Rd, Shanghai 200237, Peoples R China

年份：2016

卷号：352

期号：6283

起止页码：333

外文期刊名：SCIENCE

收录：;WOS:【SCI-EXPANDED(收录号:WOS:000373990100038)】；

基金：This work was supported by the Ontario Research Fund-Research Excellence Program, Natural Sciences and Engineering Research Council of Canada, and the Canadian Insititute for Advanced Research Bio-Inspired Solar Energy program. B. Z. acknowledges funding from China Scholarship Council/University of Toronto Joint Funding Program (201406745001), Shanghai Municipal Natural Science Foundation (14ZR1410200), and the National Natural Science Foundation of China (21503079). X.Z. acknowledges a scholarship from the China Scholarship Council (CSC) (20140625004). This work was also supported by the U.S. Department of Energy (DOE), Office of Basic Energy Science grant to the SUNCAT Center for Interface Science and Catalysis and the Laboratory-Directed Research and Development program funded through the SLAC National Accelerator Laboratory. M.G.-M. acknowledges funding from the Agency for Administration of University and Research Grants of Catalonia (AGAUR, 2013 BP-A 00464). This work has also benefited from the Hard X-ray Micro-Analysis and Spherical Grating Monochromator beamlines at CLS and the BL14W1 beamline at the Shanghai Synchrotron Radiation Facility (SSRF). B. Z. and R. C. acknowledge the CLS Post-Doctoral Student Travel Support Program. The TEM study in this work is supported by the Center for Functional Nanomaterials, which is a DOE Office of Science Facility, at Brookhaven National Laboratory under contract DE-SC0012704. E. Y. acknowledges a Fundacao de Amparo a Pesquisa do Estado de Sao Paulo-Bolsa Estagio de Pesquisa no Exterior (2014/18327-9) fellowship. E. H. S. and F.P.G.A acknowledge funding from the Connaught Global Challenge program of the University of Toronto. The authors thank D. Belanger and G. Chamoulaud at Universite du Quebec a Montreal for assistance in EQCM measurements and T.-O. Do and C.-C. Nguyen at Laval University for surface area analysis. The authors thank Y. J. Pang, X. Lan, L. N. Quan, and S. Hoogland for fruitful discussions; M. X. Liu and X. W. Gong for fabrication assistance; and R. Wolowiec and D. Kopilovic for assistance. B. Z., X. Z., J.X., M.L., C.T.D, and E.H.S. of the University of Toronto have filed provisional patent application no. 62288648 regarding the preparation of multimetal catalysts for oxygen evolution.

语种：英文

摘要：Earth-abundant first-row (3d) transition metal-based catalysts have been developed for the oxygen-evolution reaction (OER); however, they operate at overpotentials substantially above thermodynamic requirements. Density functional theory suggested that non-3d high-valency metals such as tungsten can modulate 3d metal oxides, providing nearoptimal adsorption energies for OER intermediates. We developed a room-temperature synthesis to produce gelled oxyhydroxides materials with an atomically homogeneous metal distribution. These gelled FeCoW oxyhydroxides exhibit the lowest overpotential (191 millivolts) reported at 10 milliamperes per square centimeter in alkaline electrolyte. The catalyst shows no evidence of degradation after more than 500 hours of operation. X-ray absorption and computational studies reveal a synergistic interplay between tungsten, iron, and cobalt in producing a favorable local coordination environment and electronic structure that enhance the energetics for OER.