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Room‐Temperature Activation of H 2 by a Surface Frustrated Lewis Pair
Author(s) -
Wang Lu,
Yan Tingjiang,
Song Rui,
Sun Wei,
Dong Yuchan,
Guo Jiuli,
Zhang Zizhong,
Wang Xuxu,
Ozin Geoffrey A.
Publication year - 2019
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.201904568
Subject(s) - heterolysis , lewis acids and bases , frustrated lewis pair , homolysis , chemistry , catalysis , dissociation (chemistry) , hydride , protonation , electron pair , d mannitol , hydroxide , medicinal chemistry , photochemistry , stereochemistry , radical , inorganic chemistry , organic chemistry , hydrogen , electron , mannitol , ion , physics , quantum mechanics
Surface frustrated Lewis pairs (SFLPs) have been implicated in the gas‐phase heterogeneous (photo)catalytic hydrogenation of CO 2 to CO and CH 3 OH by In 2 O 3− 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‐OH 2 + ⋅⋅⋅In‐H − . The product of the heterolysis, thought to be a protonated hydroxide Lewis base In‐OH 2 + and a hydride coordinated Lewis acid In‐H − , can react with CO 2 to form either CO or CH 3 OH. 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 In 2 O 3− 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.