Integrating theory with the nanoreactor concept to synthesize hollow carbon sphere-encapsulated PtNi alloys for enhanced H_(2) generation  

作　　者：Yufeng Wu Minwei Song Ziyi Zhao Guang-Hui Wang Changlong Wang Didier Astruc 

机构地区：[1]Institute of Circular Economy,Faculty of Materials and Manufacturing,Beijing University of Technology,Beijing,China [2]Key Laboratory of Biofuels,Qingdao Institute of Bioenergy and Bioprocess Technology,Chinese Academy of Sciences,Qingdao,China [3]ISM,UMR CNRS N°5255,Universitéde Bordeaux,Talence Cedex,France

出　　处：《Carbon Energy》2024年第7期150-162,共13页碳能源（英文）

基　　金：Financial support was received from the National Key R&D Program of China (2021YFC2902505);the start-up funding by Beijing University of Technology (Changlong Wang)。

摘　　要：The rational design of efficient bimetallic nanoparticle(NP)catalysts is challenging due to the lack of theoretical understanding of active components and insights into the mechanisms of a specific reaction.Here,we report the rational design of nanoreactors comprising hollow carbon sphere-confined PtNi bimetallic NPs(PtNi@HCS)as highly efficient catalysts for hydrogen generation via ammonia borane hydrolysis in water.Using both density functional theory calculations and molecular dynamics simulations,the effects of an active PtNi combination and the critical synergistic role of a hollow carbon shell on the molecule diffusion adsorption behaviors are explored.Kinetic isotope effects and theoretical calculations allow the clarification of the mechanism,with oxidative addition of an O-H bond of water to the catalyst surface being the rate-determining step.The remarkable catalytic activity of the PtNi@HCS nanoreactor was also utilized for successful tandem catalytic hydrogenation reactions,using in situ-generated H_(2) from ammonia borane with high efficiency.The concerted design,theoretical calculations,and experimental work presented here shed light on the rational elaboration of efficient nanocatalysts and contribute to the establishment of a circular carbon economy using green hydrogen.

关 键 词：ammonia borane hydrogen NANOALLOY NANOREACTOR solid catalyst 

分 类 号：TB383[一般工业技术—材料科学与工程]