4.8 Article

High-Performance and Long-Lived Pd Nanocatalyst Directed by Shape Effect for CO Oxidative Coupling to Dimethyl Oxalate

Journal

ACS CATALYSIS
Volume 3, Issue 2, Pages 118-122

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/cs300759h

Keywords

CO oxidative coupling to dimethyl oxalate; Pd nanocatalyst; shape effect; wet impregnation-solution chemical reduction method

Funding

  1. 973 Program [2011CBA00505]
  2. National Key Technology RD Program [2012BAE06B08]
  3. NSF of China [90922035, 21003126]
  4. CAS [KJCX2.YW.M10]
  5. NSF of Fujian province

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We synthesized monodisperse Pd nanocrystals with exposed (111) and (100) facets through preferentially oriented facet growth technology. We then supported them on alpha-Al2O3 as catalysts for application in CO oxidative coupling to dimethyl oxalate (DMO) and find, for the first time, that the (111) facets of Pd nanocrystals are active planes for CO oxidative coupling to DMO. This conclusion is based on experiment results, reaction mechanism, and density functional theory calculation. Directed by this shape effect, a high-performance and long-lived nanocatalyst with much lower Pd load for CO oxidative coupling to DMO was successfully prepared by a new wet impregnation-solution chemical reduction method, which can well control the exposure of (111) facets and sizes of Pd nanocrystals.

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