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[期刊论文]

Room-Temperature Activation of H2 by a Surface Frustrated Lewis Pair

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author:

Wang, L. (Wang, L..) [1] | Yan, T. (Yan, T..) [2] | Song, R. (Song, R..) [3] | Unfold

Indexed by:

Scopus

Abstract:

Surface frustrated Lewis pairs (SFLPs) have been implicated in the gas-phase heterogeneous (photo)catalytic hydrogenation of CO2 to CO and CH3OH by In2O3−x(OH)y. A key step in the reaction pathway is envisioned to be the heterolysis of H2 on a proximal Lewis acid–Lewis base pair, the SFLP, the chemistry of which is described as In⋅⋅⋅In-OH + H2 → In-OH2+⋅⋅⋅In-H−. The product of the heterolysis, thought to be a protonated hydroxide Lewis base In-OH2+ and a hydride coordinated Lewis acid In-H−, can react with CO2 to form either CO or CH3OH. While the experimental and theoretical evidence is compelling for heterolysis of H2 on the SFLP, all conclusions derive from indirect proof, and direct observation remains lacking. Unexpectedly, we have discovered rhombohedral In2O3−x(OH)y can enable dissociation of H2 at room temperature, which allows its direct observation by several analytical techniques. The collected analytical results lean towards the heterolysis rather than the homolysis reaction pathway. © 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

Keyword:

gas-phase reactions; heterolytic H2 dissociation; indium oxide; surface chemistry; surface frustrated Lewis pair

Community:

  • [ 1 ] [Wang, L.]Department of Chemistry, University of Toronto, 80 St. George Street, Toronto, ON M5S3H6, Canada
  • [ 2 ] [Yan, T.]Department of Chemistry, University of Toronto, 80 St. George Street, Toronto, ON M5S3H6, Canada
  • [ 3 ] [Yan, T.]College of Chemistry and Chemical Engineering, Qufu Normal University, Qufu, Shandong 273165, China
  • [ 4 ] [Song, R.]Department of Chemistry, University of Toronto, 80 St. George Street, Toronto, ON M5S3H6, Canada
  • [ 5 ] [Song, R.]International Research Center for Renewable Energy & State Key Laboratory of Multiphase Flow in Power Engineering, Xi'an Jiaotong University, Xi'an, Shanxi 710049, China
  • [ 6 ] [Sun, W.]Department of Chemistry, University of Toronto, 80 St. George Street, Toronto, ON M5S3H6, Canada
  • [ 7 ] [Dong, Y.]Department of Chemistry, University of Toronto, 80 St. George Street, Toronto, ON M5S3H6, Canada
  • [ 8 ] [Guo, J.]Department of Chemistry, University of Toronto, 80 St. George Street, Toronto, ON M5S3H6, Canada
  • [ 9 ] [Guo, J.]Department of Chemistry, Nankai University, Tianjin, 300071, China
  • [ 10 ] [Zhang, Z.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350108, China
  • [ 11 ] [Wang, X.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350108, China
  • [ 12 ] [Ozin, G.A.]Department of Chemistry, University of Toronto, 80 St. George Street, Toronto, ON M5S3H6, Canada

Reprint 's Address:

  • [Yan, T.]Department of Chemistry, University of Toronto, 80 St. George Street, Canada

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Source :

Angewandte Chemie - International Edition

ISSN: 1433-7851

Year: 2019

Issue: 28

Volume: 58

Page: 9501-9505

1 2 . 9 5 9

JCR@2019

1 6 . 1 0 0

JCR@2023

ESI HC Threshold:184

JCR Journal Grade:1

CAS Journal Grade:1

Cited Count:

WoS CC Cited Count:

30 Days PV: 0

Affiliated Colleges:

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