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Regulating Peripheral Nitrogen Dopants in Single-Atom Catalysts to Enhance Propane Dehydrogenation
Fenfei Wei1,2, Liru Cao3,4, Bingqing Ge1
1State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350002, China.
Peripheral nitrogen dopants in single-atom catalysts (SACs) significantly impact propane dehydrogenation (PDH) activity and selectivity. Stochastic doping models reveal that farther nitrogen dopants enhance Ir1 SAC performance for PDH.
Area of Science:
- Heterogeneous Catalysis
- Materials Science
- Computational Chemistry
Background:
- Dopants near metal sites in single-atom catalysts (SACs) affect properties.
- The role of distant dopants in SACs is not well understood.
Purpose of the Study:
- Investigate the effect of peripheral nitrogen dopant distance on Ir1 SACs for propane dehydrogenation (PDH).
- Elucidate the working mechanism of distant dopants in SACs.
Main Methods:
- Density functional theory (DFT)-driven studies.
- Stochastic doping models.
- Experimental verification.
Main Results:
- Dopant distance influences reaction energy changes in Ir1 SACs.
- Increased nitrogen in farther shells enhances Ir1 activity and propene selectivity.
- Modulation of Ir1 d-band center by dopants optimizes binding energies of intermediates.
Conclusions:
- Distant dopants play a crucial role in tuning SAC performance.
- Stochastic doping engineering offers a strategy for optimizing heterogeneous catalysts.
- Understanding dopant states is key for designing advanced catalysts.
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