title: Explaining the Size Dependence in Platinum-Nanoparticle-Catalyzed Hydrogenation Reactions.
abstract: Hydrogenation reactions are industrially important reactions that typically require unfavorably high H2pressure and temperature for many functional groups. Herein we reveal surprisingly strong size-dependent activity of Pt nanoparticles (PtNPs) in catalyzing this reaction. Based on unambiguous spectral analyses, the size effect has been rationalized by the size-dependent d-band electron structure of the PtNPs. This understanding enables production of a catalyst with size of 1.2 nm, which shows a sixfold increase in turnover frequency and 28-fold increase in mass activity in the regioselective hydrogenation of quinoline, compared with PtNPs of 5.3 nm, allowing the reaction to proceed under ambient conditions with unprecedentedly high reaction rates. The size effect and the synthesis strategy developed herein may provide a general methodology in the design of metal-nanoparticle-based catalysts for a broad range of organic syntheses.
authors.affiliation: Frontier Institute of Science and Technology, and State Key Laboratory for Mechanical Behavior of Materials, Xi'an Jiaotong University, Xi'an, Shaanxi, 710054, China.
authors.forename: Licheng
authors.initials: L
authors.lastname: Bai
authors.affiliation: Frontier Institute of Science and Technology, and State Key Laboratory for Mechanical Behavior of Materials, Xi'an Jiaotong University, Xi'an, Shaanxi, 710054, China.|Department of Chemistry, University of California, Riverside, Riverside, CA, 92521, USA.
authors.forename: Xin
authors.initials: X
authors.lastname: Wang
authors.affiliation: School of Chemical Engineering and Technology, Xi'an Jiaotong University, Xi'an, Shaanxi, 710049, China.
authors.forename: Qiang
authors.initials: Q
authors.lastname: Chen
authors.affiliation: Advanced Light Source Division, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720, USA.
authors.forename: Yifan
authors.initials: Y
authors.lastname: Ye
authors.affiliation: Department of Materials and Environmental Chemistry, Stockholm University, Stockholm, 10691, Sweden.
authors.forename: Haoquan
authors.initials: H
authors.lastname: Zheng
authors.affiliation: Advanced Light Source Division, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720, USA.
authors.forename: Jinghua
authors.initials: J
authors.lastname: Guo
authors.affiliation: Department of Chemistry, University of California, Riverside, Riverside, CA, 92521, USA.
authors.forename: Yadong
authors.identifier: 0000-0003-0218-3042
authors.initials: Y
authors.lastname: Yin
authors.affiliation: Frontier Institute of Science and Technology, and State Key Laboratory for Mechanical Behavior of Materials, Xi'an Jiaotong University, Xi'an, Shaanxi, 710054, China.
authors.forename: Chuanbo
authors.identifier: 0000-0003-3429-3473
authors.initials: C
authors.lastname: Gao
keywords: d-band electron structure; heterogeneous catalysis; hydrogenation reactions; platinum nanoparticles; size effects