摘要
Bimetallic palladium-gold （PdAu） catalysts have better catalytic performance than monometallic catalysts for many applications. PdAu catalysts with controlled nanostructures and enhanced activi- ties 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 hydro- dech/orination 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 mOITcE mOled-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^-1s^-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,
在许多催化应用中双金属的Pd Au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Pd Au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Pd Au/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H_2还原的过程后,所制得的Pd Au/C催化剂活性最高,初始转化频率(TOF)为34.0×10^(–2) mol_(TCE) mol^(–1)Pd s^(–1),是单金属1.0 wt%Pd/C催化剂TOF(2.2×10^(–2) mol_(TCE) mol^(–1)Pd 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 oC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.
基金
supported by the National Science Foundation,United States(EEC-0647452)
the Welch Foundation(C-1676)~~
