文献类型：期刊文献

英文题名：Revealing the Sudden Alternation in Pt@h-BN Nanoreactors for Nearly 100% CO2-to-CH4 Photoreduction

作者：Bi, Wei[1];Hu, Yanjie[1];Jiang, Hao[1];Zhang, Ling[1];Li, Chunzhong[1]

机构：[1]East China Univ Sci & Technol, Sch Mat Sci & Engn, Minist Educ, Key Lab Ultrafine Mat,Shanghai Engn Res Ctr Hiera, Shanghai 200237, Peoples R China

年份：2021

卷号：31

期号：29

外文期刊名：ADVANCED FUNCTIONAL MATERIALS

收录：;EI(收录号：20212010355533);WOS:【SCI-EXPANDED(收录号:WOS:000649439800001)】；

基金：This work was supported by the National Natural Science Foundation of China (21978088, 91534202, 51673063), Shanghai Technology Research Leader (20XD1433600), the Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutes of High Learning, the Basic Research Program of Shanghai (17JC1402300), the Social Development Program of Shanghai (17DZ1200900), the Shanghai City Board of education research and innovation project, and the Fundamental Research Funds for the Central Universities (222201718002). Additional support was provided by Feringa Nobel Prize Scientist Joint Research Center.

语种：英文

外文关键词：100% CO; (2)‐ to‐ CH; (4); confinement effects; photocatalytic CO; (2) reduction; Pt@h‐ BN nanoreactors; orderly relay reactions

摘要：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.