title: PtNi/NiO Clusters Coated by Hollow Sillica: Novel Design for Highly Efficient Hydrogen Production from Ammonia-Borane.
abstract: Ammonia-borane (NH3·BH3; AB) has been considered as an excellent chemical material for hydrogen storage. However, developing highly efficient catalysts for continuous hydrogen generation from AB is still a challenge for future fuel cell applications. The combination of Pt with Ni is an effective strategy to achieve active bimetallic nanocatalyst, and the particle size has proved to play a crucial role in determining its final activity. However, the synthesis of PtNi bimetallic catalyst in the size of highly dispersed clusters has always been a challenge. In this report, PtNi/NiO clusters coated by small-sized hollow silica (R-PtNi/NiO@SiO2) were designed for efficient hydrogen generation from the hydrolysis of ammonia-borane. The newly designed catalysis system showed extremely high activity with the initial turnover frequency value reaching 1240.3 mol of H2·mol-1of Pt·min-1, which makes it one the most active Pt-based catalysts for this reaction. Detailed characterization by means of scanning transmission electron microscopy, X-ray photoelectron spectroscopy, energy-dispersive X-ray spectroscopy element mapping, etc. revealed that the excellent performance of R-PtNi/NiO@SiO2is derived from the highly dispersed PtNi/NiO clusters and the reduction of extra Pt4+on the surface of PtNi/NiO clusters to Pt0at relatively low temperature.
authors.affiliation: State Key Laboratory of Fine Chemicals, Dalian University of Technology , Dalian 116024, People's Republic of China.
authors.forename: Yuzhen
authors.identifier: http://orcid.org/0000-0002-2133-1509
authors.initials: Y
authors.lastname: Ge
authors.affiliation: State Key Laboratory of Fine Chemicals, Dalian University of Technology , Dalian 116024, People's Republic of China.
authors.forename: Wanyue
authors.initials: W
authors.lastname: Ye
authors.affiliation: State Key Laboratory of Fine Chemicals, Dalian University of Technology , Dalian 116024, People's Republic of China.
authors.forename: Zameer Hussain
authors.identifier: http://orcid.org/0000-0002-8249-6403
authors.initials: ZH
authors.lastname: Shah
authors.affiliation: State Key Laboratory of Fine Chemicals, Dalian University of Technology , Dalian 116024, People's Republic of China.
authors.forename: Xijie
authors.initials: X
authors.lastname: Lin
authors.affiliation: State Key Laboratory of Fine Chemicals, Dalian University of Technology , Dalian 116024, People's Republic of China.
authors.forename: Rongwen
authors.identifier: http://orcid.org/0000-0002-2210-3380
authors.initials: R
authors.lastname: Lu
authors.affiliation: State Key Laboratory of Fine Chemicals, Dalian University of Technology , Dalian 116024, People's Republic of China.
authors.forename: Shufen
authors.initials: S
authors.lastname: Zhang
keywords: ammonia−borane; heterogeneous catalysis; hollow silica; hydrogen storage; platinum−nickel cluster