Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 58, Issue 28, Pages 9501-9505Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201904568
Keywords
gas-phase reactions; heterolytic H-2 dissociation; indium oxide; surface chemistry; surface frustrated Lewis pair
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Funding
- Ontario Ministry of Research and Innovation (MRI)
- Ministry of Economic Development, Employment and Infrastructure (MEDI)
- Ministry of the Environment and Climate Change's (MOECC)
- Best in Science (BIS) Award
- Ontario Center of Excellence (OCE) Solutions 2030 Challenge Fund
- Low Carbon Innovation Fund (LCIF), Imperial Oil
- University of Toronto Connaught Innovation Fund (CIF)
- Connaught Global Challenge (CGC) Fund
- Natural Sciences and Engineering Research Council of Canada (NSERC)
- National Natural Science Foundation of China [21872081]
- Natural Science Foundation of Shandong Province [ZR2016BM04]
- Open Project Program of the State Key Laboratory of Photocatalysis on Energy and Environment [SKLPEE-KF201711]
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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 H-2 on a proximal Lewis acid-Lewis base pair, the SFLP, the chemistry of which is described as In...In-OH + H-2 -> 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 H-2 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 H-2 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.
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