4.8 Article

MOF-Confined Sub-2 nm Atomically Ordered Intermetallic PdZn Nanoparticles as High-Performance Catalysts for Selective Hydrogenation of Acetylene

Journal

ADVANCED MATERIALS
Volume 30, Issue 33, Pages -

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.201801878

Keywords

intermetallics; MOF-confined; sub-2 nm

Funding

  1. National Key R&D Program of China [2017YFA0700101, 2016YFA0202801]
  2. National Natural Science Foundation of China [21573119, 21590792, 21521091, 21390393, U1463202, 21473199]
  3. Beijing Municipal Science & Technology Commission
  4. Beijing Natural Science Foundation [2184097]
  5. Chinese Academy of Sciences

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Controllable synthesis of ultrasmall atomically ordered intermetallic nanoparticles is a challenging task, owing to the high temperature commonly required for the formation of intermetallic phases. Here, a metal-organic framework (MOF)-confined co-reduction strategy is developed for the preparation of sub-2 nm intermetallic PdZn nanoparticles, by employing the well-defined porous structures of calcinated ZIF-8 (ZIF-8C) and an in situ co-reduction therein. HAADF-STEM, HRTEM, and EDS characterizations reveal the homogeneous dispersion of these sub-2 nm intermetallic PdZn nanoparticles within the ZIF-8C frameworks. XRD, XPS, and EXAFS measurements further confirm the atomically ordered intermetallic phase nature of these sub-2 nm PdZn nanoparticles. Selective hydrogenation of acetylene evaluation results show the excellent catalytic properties of the sub-2 nm intermetallic PdZn, which result from the energetically more favorable path for acetylene hydrogenation and ethylene desorption over the ultrasmall particles than over larger-sized intermetallic PdZn as revealed by density functional theory (DFT) calculations. Moreover, this protocol is also extendable for the preparation of sub-2 nm intermetallic PtZn nanoparticles and is expected to provide a novel methodology in synthesizing ultrasmall atomically ordered intermetallic nanomaterials by rationally functionalizing MOFs.

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