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yexuqing

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[交流] 用新催化剂可从酸水制备氢气 已有1人参与

Science 10 February 2012:
Vol. 335 no. 6069 pp. 698-702
DOI: 10.1126/science.1215868
Report


A Molecular MoS2 Edge Site Mimic for Catalytic Hydrogen Generation
Hemamala I. Karunadasa1,2, Elizabeth Montalvo1, Yujie Sun1,2, Marcin Majda1, Jeffrey R. Long1,3,*, Christopher J. Chang1,2,4,*
+ Author Affiliations

1Department of Chemistry, University of California, Berkeley, CA 94720, USA.
2Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.
3Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.
4Howard Hughes Medical Institute, University of California, Berkeley, CA 94720, USA.
↵*To whom correspondence should be addressed. E-mail: chrischang@berkeley.edu (C.J.C.); jrlong@berkeley.edu (J.R.L.)
Abstract
Inorganic solids are an important class of catalysts that often derive their activity from sparse active sites that are structurally distinct from the inactive bulk. Rationally optimizing activity is therefore beholden to the challenges in studying these active sites in molecular detail. Here, we report a molecule that mimics the structure of the proposed triangular active edge site fragments of molybdenum disulfide (MoS2), a widely used industrial catalyst that has shown promise as a low-cost alternative to platinum for electrocatalytic hydrogen production. By leveraging the robust coordination environment of a pentapyridyl ligand, we synthesized and structurally characterized a well-defined MoIV-disulfide complex that, upon electrochemical reduction, can catalytically generate hydrogen from acidic organic media as well as from acidic water.

Received for publication 27 October 2011.
Accepted for publication 22 December 2011.
http://www.sciencemag.org/conten ... 0-85f7-d01a7c323a0e

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