4.8 Article

Single-Molecule Nanocatalysis Reveals Facet-Dependent Catalytic Kinetics and Dynamics of Pallidium Nanoparticles

Journal

ACS CATALYSIS
Volume 7, Issue 4, Pages 2967-2972

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acscatal.7b00087

Keywords

Pd nanoparticles; single molecule; nanocatalysis; fluorescence microscopy; shape effect

Funding

  1. National Basic Research Program of China (973 Program) [2014CB932700]
  2. National Natural Science Foundation of China [U1601211, 21633008, 21422307, 21433003, 21573215, 21503212, 21573206]
  3. the Recruitment Program of Global youth Experts of China
  4. Science and Technology Innovation Foundation of Jilin Province for Talents Cultivation [20160519005JH]
  5. Jilin Youth foundation [20160520137JH]

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By studying the nanocatalysis of individual Pd nanoparticles (Pd NPs) in two shapes (cube with (100) facet and octahedron with (111) facet) with single-turnover resolution, the facet-dependent activities and dynamics were apparently observed. The results indicate that Pd octahedrons possess higher intrinsic catalytic activity per site than Pd nanocubes. Within a competitive Langmuir-Hinshelwood mechanism, the facet-dependent activities are derived at single-particle level, and the facet-dependent adsorption behaviors of substrate molecules on Pd(111) and Pd(100) are revealed and clarified by theoretical calculation. Furthermore, the facet-dependent restructuring behaviors of the particle surfaces were also observed. This study gives deeper insight into Pd-based nanocatalysts.

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