催化学报

催化学报 ›› 2016, Vol. 37 ›› Issue (10): 1776-1786.DOI: 10.1016/S1872-2067(16)62530-5

• 论文 • 上一篇    下一篇

金掺杂对碳负载钯催化还原性能的促进作用

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 莱斯大学化工与生物分子工程系, 休斯顿 77005, 美国;
    b 莱斯大学化学系, 休斯顿 77005, 美国;
    c 阿贡国家实验室化工科学与工程部, 阿贡IL 60439, 美国;
    d 普渡大学化工系, 西拉斐特, 美国;
    e 莱斯大学土木与环境工程系, 休斯顿 77005, 美国;
    f 莱斯大学材料科学与纳米工程系, 休斯顿 77005, 美国
  • 收稿日期:2016-05-28 修回日期:2016-08-14 出版日期:2016-10-21 发布日期:2016-10-22
  • 通讯作者: Michael S. Wong
  • 基金资助:

    美国国家科学基金会（EEC-0647452）；维尔许基金（C-1676）.

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).

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摘要：

在许多催化应用中双金属的PdAu催化剂性能优于单金属催化剂.科研人员对具有可控纳米结构和高活性的PdAu催化剂进行了广泛的研究，但该催化剂的制备需要多步且通常步骤复杂.本文仅通过浸渍和焙烧制得了Au掺杂的负载型Pd催化剂，所得PdAu/C催化剂用于室温水相三氯乙烯加氢脱氯反应.当Pd和Au负载量分别为1.0 wt%和1.1 wt%时，在经过干燥、空气处理和H2还原的过程后，所制得的PdAu/C催化剂活性最高，初始转化频率（TOF）为34.0×10-2 molTCE molPd-1 s-1，是单金属1.0 wt% Pd/C催化剂TOF（2.2×10-2 molTCE molPd-1 s-1）的15倍以上.X射线吸收光谱结果表明，金的加入避免了400℃焙烧时Pd的氧化.本文还提出了可能的催化剂纳米结构演变路径，以解释所观察到的催化现象.

关键词: 双金属催化剂, 钯, 金, 纳米结构, X射线吸收光谱, 扩展X射线吸收精细结构, 加氢脱氯, 三氯乙烯

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