Journal
SMALL
Volume 13, Issue 31, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.201701354
Keywords
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Categories
Funding
- 973 Program [2014CB848900]
- NSFC [21471141, U1532135, 21601173, 21573212]
- CAS Key Research Program of Frontier Sciences [QYZDB-SSW-SLH018]
- CAS Interdisciplinary Innovation Team
- Recruitment Program of Global Experts
- CAS Hundred Talent Program
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Adsorption and activation of molecules on a surface holds the key to heterogeneous catalysis toward aerobic oxidative reactions. To achieve high catalytic activities, a catalyst surface should be rationally tailored to interact with both organic substrates and oxygen molecules. Here, a facile bottom-up approach to defective tungsten oxide hydrate (WO3 center dot H2O) nanosheets that contain both surface defects and lattice water is reported. The defective WO3 center dot H2O nanosheets exhibit excellent catalytic activity for aerobic coupling of amines to imines. The investigation indicates that the oxygen vacancies derived from surface defects supply coordinatively unsaturated sites to adsorb and activate oxygen molecules, producing superoxide radicals. More importantly, the Bronsted acid sites from lattice water can contribute to enhancing the adsorption and activation of alkaline amine molecules. The synergistic effect of oxygen vacancies and Bronsted acid sites eventually boosts the catalytic activity, which achieves a kinetic rate constant of 0.455 h(-1) and a turnover frequency of 0.85 h(-1) at 2 h, with the activation energy reduced to approximate to 35 kJ mol(-1). This work provides a different angle for metal oxide catalyst design by maneuvering subtle structural features, and highlights the importance of synergistic effects to heterogeneous catalysts.
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