期刊
ADVANCED FUNCTIONAL MATERIALS
卷 31, 期 29, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.202010780
关键词
100% CO; (2)‐ to‐ CH; (4); confinement effects; photocatalytic CO; (2) reduction; Pt@h‐ BN nanoreactors; orderly relay reactions
类别
资金
- National Natural Science Foundation of China [21978088, 91534202, 51673063]
- Shanghai Technology Research Leader [20XD1433600]
- Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutes of High Learning
- Basic Research Program of Shanghai [17JC1402300]
- Social Development Program of Shanghai [17DZ1200900]
- Shanghai City Board of education research and innovation project
- Fundamental Research Funds for the Central Universities [222201718002]
- Feringa Nobel Prize Scientist Joint Research Center
This study focuses on the development of efficient photocatalysts with high selectivity through the synthesis of Pt@h-BN nanoreactors. Detailed experimental and simulation calculations reveal the confinement effect and the change in reaction sites play vital roles in the catalytic reaction process.
How to develop an efficient photocatalyst with high activity and high selectivity is the biggest challenge limiting the application of photocatalysis. A reasonable design of the nanoreactor model is an effective strategy. Herein, a series of Pt nanoparticles coated with hexagonal boron nitride (Pt@h-BN) nanoreactors highly dispersed on a photochemically inert carrier, Al2O3 substrate, are synthesized. The results show that as the number of h-BN coating layers increases, the selectivity of photocatalysis is altered from nearly 100% CO2-to-CO to nearly 100% CO2-to-CH4, and the optimized space-time yield of CH4 is up to 184.7 mu mol g((Pt))(-1) h(-1) with three-layer coating. The in situ characterizations reveal the cleavage of the CO on Pt to be the rate determining step and the existence of the key intermediate CO2- species on the surface of Pt@h-BN facilitates CH4 formation. Notably, combined with detailed simulation calculations, this work reveals that the confinement effect in Pt@h-BN attributes the electrons mobility behavior and alleviate the interaction of CO-Pt. What is more, the change of the reaction site is the essence for the sudden alternation. This work will bring a new insight to the selective catalysis of noble metals in the gas-solid phase.
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