Chinese Journal of Catalysis ›› 2016, Vol. 37 ›› Issue (10): 1776-1786.DOI: 10.1016/S1872-2067(16)62530-5

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Gold-doping of carbon-supported palladium improves reduction catalysis

Yu-Lun Fanga, Kimberly N. Hecka, Zhun Zhaoa, Lori A. Pretzerb, Neng Guoc, Tianpin Wuc, Jeffrey T. Millerd, Michael S. Wonga,b,e,f   

  1. a Department of Chemical and Biomolecular Engineering, Rice University, 6100 S. Main Street, Houston, TX 77005, USA;
    b Department of Chemistry, Rice University, 6100 S. Main Street, Houston, TX 77005, USA;
    c Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 S. Cass Avenue, Argonne, IL 60439, USA;
    d Department of Chemical Engineering, Purdue University, 480 Stadium Mall Drive West Lafayette, IN 47907, USA;
    e Department of Civil and Environmental Engineering, Rice University, 6100 S. Main Street, Houston, TX 77005, USA;
    f Department of Materials Science and NanoEngineering, Rice University, 6100 S. Main Street, Houston, TX 77005, USA
  • Received:2016-05-28 Revised:2016-08-14 Online:2016-10-21 Published:2016-10-22
  • Contact: Michael S. Wong
  • Supported by:

    This work was supported by the National Science Foundation, United States (EEC-0647452) and the Welch Foundation (C-1676).

Abstract:

Bimetallic palladium-gold (PdAu) catalysts have better catalytic performance than monometallic catalysts for many applications. PdAu catalysts with controlled nanostructures and enhanced activities have been extensively studied but their syntheses require multiple and occasionally complicated steps. In this work, we demonstrated that supported PdAu catalysts could be simply prepared by doping a supported Pd catalyst with gold through wet impregnation and calcination. Resulting PdAu-on-carbon (PdAu/C) catalysts were tested for the room-temperature, aqueous-phase hydrodechlorination of trichloroethene. The most active PdAu/C catalyst (Pd 1.0 wt%, Au 1.1 wt%, dried/air/H2 process) had an initial turnover frequency (TOF) of 34.0×10-2 molTCE molPd-1 s-1, which was >15 times higher than monometallic Pd/C (Pd 1.0 wt%, initial TOF of 2.2×10-2 molTCE molPd-1 s-1). Through X-ray absorption spectroscopy, the gold kept Pd from oxidizing under calcination at 400℃. Probable nanostructure evolution pathways are proposed to explain the observed catalysis.

Key words: Bimetallic catalyst, Palladium, Gold, Nanostructures, X-ray absorption spectroscopy, Extended X-ray absorption fine structure, Hydrodechlorination, Trichloroethene