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      Active sites for CO2 hydrogenation to methanol on Cu/ZnO catalysts.

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          Abstract

          The active sites over commercial copper/zinc oxide/aluminum oxide (Cu/ZnO/Al2O3) catalysts for carbon dioxide (CO2) hydrogenation to methanol, the Zn-Cu bimetallic sites or ZnO-Cu interfacial sites, have recently been the subject of intense debate. We report a direct comparison between the activity of ZnCu and ZnO/Cu model catalysts for methanol synthesis. By combining x-ray photoemission spectroscopy, density functional theory, and kinetic Monte Carlo simulations, we can identify and characterize the reactivity of each catalyst. Both experimental and theoretical results agree that ZnCu undergoes surface oxidation under the reaction conditions so that surface Zn transforms into ZnO and allows ZnCu to reach the activity of ZnO/Cu with the same Zn coverage. Our results highlight a synergy of Cu and ZnO at the interface that facilitates methanol synthesis via formate intermediates.

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          Author and article information

          Journal
          Science
          Science (New York, N.Y.)
          American Association for the Advancement of Science (AAAS)
          1095-9203
          0036-8075
          Mar 24 2017
          : 355
          : 6331
          Affiliations
          [1 ] Chemistry Division, Brookhaven National Laboratory, Upton, NY 11973, USA.
          [2 ] Facultad de Ciencias, Universidad Central de Venezuela, Caracas 1020-A, Venezuela.
          [3 ] Chemistry Division, Brookhaven National Laboratory, Upton, NY 11973, USA. jgchen@columbia.edu rodrigez@bnl.gov pingliu3@bnl.gov.
          [4 ] Department of Chemical Engineering, Columbia University, New York, NY 10027, USA.
          [5 ] Department of Chemistry, State University of New York-Stony Brook, Stony Brook, NY 11790, USA.
          Article
          355/6331/1296
          10.1126/science.aal3573
          28336665
          5ba84908-8b7d-497f-8f4c-ba4f659c6d9f
          History

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