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Updated: Jun 13, 2025

Tuning the Acidity of Pt/ CNTs Catalysts for Hydrodeoxygenation of Diphenyl Ether
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Crystal Facet Enhanced Dynamic Stability and Reactivity of Undercoordinated Pt1-TiO2 Single Atom Species for Methane
Qi Wang1,2, Qingqing Gu1, Aiqin Wang1
1CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China.
None:
The influence of crystal facets of the support on the dynamic evolution of single-atom catalysts (SACs) during real reactions remains elusive. Herein, we report a crystal facet mediated dynamic evolution and reactivity of Pt1-TiO2 SACs for methane oxidation. Under reaction conditions, the TiO2(001) favored dynamic formation of undercoordinated Ptδ+ species (0 < δ < 2) in association with Ti3+-Ov moieties (Ptδ+-Ov-Ti3+) for high activity, whereas TiO2(101) surface stabilized Pt4+ species with saturated Pt-O coordination showing nearly no activity. Both the crystal facet of the support and the reaction environment are crucial for spontaneous formation of Ptδ+-Ov-Ti3+ species during reaction, showing unique dynamic stability that is different from their thermal/reduction stability. The enhanced acidity of Ptδ+-Ov-Ti3+ facilitates C-H activation and O2 dissociation for methane oxidation. This work elucidates crystal facet enhanced stability and reactivity of Ptδ+-Ov-Ti3+ species during reaction and paves a new route for the rational design of SACs based on their dynamic stability.
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