Theoretical Study of the Hydrogen Absorption Mechanism into a Palladium Nanocube Coated with a Metal-Organic Framework

Yusuke Nanba, Tatsuki Tsutsumi, Takayoshi Ishimoto, Michihisa Koyama

    Research output: Contribution to journalArticlepeer-review

    8 Citations (Scopus)

    Abstract

    We analyzed theoretically the hydrogen absorption properties and kinetics into Pd nanocubes coated with copper(II) 1,3,5-benzenetricarboxylate (HKUST-1), which is a type of metal-organic framework, using density functional theory. We prepared an interface model consisting of the Pd(100) surface and Cu-edged HKUST-1 structure and calculated the hydrogen adsorption and absorption energies in a Pd nanocube model. To discuss the kinetics of the hydrogen absorption, we also evaluated the hydrogen diffusion barrier near the interface. Compared with bare Pd, the hydrogen diffusion barrier from the surface to the subsurface decreased. We found that the adsorption of HKUST-1 on the Pd nanocube leads to chemical and steric effects for the diffusion rate increase of hydrogen. As a chemical effect, hydrogen adsorption was destabilized by the change of electronic structure of the Pd surface because of the atomic charge displacement between the Pd and Cu atoms in HKUST-1. As a steric effect, a new hydrogen diffusion path from the unique Pd5Cu octahedral site was created. (Graph Presented).

    Original languageEnglish
    Pages (from-to)14611-14617
    Number of pages7
    JournalJournal of Physical Chemistry C
    Volume121
    Issue number27
    DOIs
    Publication statusPublished - Jul 13 2017

    All Science Journal Classification (ASJC) codes

    • Electronic, Optical and Magnetic Materials
    • Energy(all)
    • Physical and Theoretical Chemistry
    • Surfaces, Coatings and Films

    Fingerprint Dive into the research topics of 'Theoretical Study of the Hydrogen Absorption Mechanism into a Palladium Nanocube Coated with a Metal-Organic Framework'. Together they form a unique fingerprint.

    Cite this