期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 57, 期 13, 页码 3327-3331出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201710791
关键词
ab initio simulations; gold nanoparticles; Grotthuss-type proton diffusion; heterogeneous catalysis; titania
资金
- Cluster of Excellence RESOLV - Deutsche Forschungsgemeinschaft [EXC 1069]
Gold/titania catalysts are widely used for key reactions, notably including the selective oxidation of alcohols in the liquid phase. Our large-scale abinitio simulations disclose that the liquid-phase reaction mechanism is distinctly different from that in the gas phase because of active participation of water molecules. While concerted charge transfers related to O-2 splitting and abstraction of both protonic and hydridic hydrogens are enforced under dry conditions, stepwise charge transfer is preferred in the condensed phase. Dissociation of reactive water molecules and subsequent Grotthuss migration of protonic defects, H+(aq), allows for such a decoupling of the oxidation process, both in time and space. It is expected that these observations are paradigmatic for heterogeneous catalysis in aqueous phases.
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