催化学报

催化学报 ›› 2017, Vol. 38 ›› Issue (2): 207-216.DOI: 10.1016/S1872-2067(16)62569-X

• 论文 • 上一篇    下一篇

四氧化三钴负载金钯纳米催化剂催化消除甲苯和邻二甲苯

王治伟a, 刘雨溪a, 杨涛b, 邓积光a, 谢少华a, 戴洪兴a   

  1. a 北京工业大学环境与能源工程学院化学化工系, 绿色催化与分离北京市重点实验室, 区域大气复合污染防治北京市重点实验室, 催化化学与纳米科学实验室, 北京 100124;
    b 阿威罗大学机械工程系, 阿威罗3810-193, 葡萄牙
  • 收稿日期:2016-09-17 修回日期:2016-10-27 出版日期:2017-02-18 发布日期:2017-03-14
  • 通讯作者: Jiguang Deng,Tel:+86-10-67396118;Fax:+86-10-67391983;E-mail:jgdeng@bjut.edu.cn;Hongxing Dai,Tel:+86-10-67396118;Fax:+86-10-67391983;E-mail:hxdai@bjut.edu.cn
  • 基金资助:

    国家自然科学基金（21377008，21477005，U1507108）；国家高技术研究发展计划（2015AA034603）；北京市科技新星计划（Z141109001814106）；北京市教委科技计划（KM201410005008）.

Catalytic performance of cobalt oxide-supported gold-palladium nanocatalysts for the removal of toluene and o-xylene

Zhiwei Wanga, Yuxi Liua, Tao Yangb, Jiguang Denga, Shaohua Xiea, Hongxing Daia   

  1. a Beijing Key Laboratory for Green Catalysis and Separation, Key Laboratory of Beijing on Regional Air Pollution Control, and Laboratory of Catalysis Chemistry and Nanoscience, Department of Chemistry and Chemical Engineering, College of Environmental and Energy Engineering, Beijing University of Technology, Beijing 100124, China;
    b Mechanical Engineering Department, University of Aveiro, 3810-193 Aveiro, Portugal
  • Received:2016-09-17 Revised:2016-10-27 Online:2017-02-18 Published:2017-03-14
  • Contact: 10.1016/S1872-2067(16)62569-X
  • Supported by:

    This work was supported by the National Natural Science Foundation of China (21377008, 21477005, U1507108), National High Technology Research and Development Program of China (2015AA034603), Beijing Nova Program (Z141109001814106), and Natural Science Foundation of Beijing Municipal Commission of Education (KM201410005008).

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1016

被引次数

1

摘要：

挥发性有机物（VOCs，例如甲苯和二甲苯）不仅危害人身健康，而且对大气环境造成严重污染.由于去除效率高、无二次污染以及耗能低等优点，催化氧化法被认为是消除VOCs的有效方法之一.该方法的关键是高效催化剂的研发.由于具有良好的低温催化氧化性能，过渡金属氧化物负载的贵金属催化剂备受关注.相比于单组分贵金属负载型催化剂，双组分贵金属负载型催化剂的催化活性、水热稳定性能和抗硫中毒性能均有显著提高.
本文采用熔融盐法和聚乙烯醇保护的硼氢化钠还原法制备了八面体状Co3O4负载的AuPd（x（AuPdy）/Co3O4；AuPd负载量x=（0.18，0.47，0.97）wt%；Pd/Au摩尔比y=1.85，1.93，1.92）合金纳米催化剂.采用X射线衍射、扫描电子显微镜、透射电子显微镜、选区电子衍射、氢气程序升温还原、氧气程序升温脱附和X射线光电子衍射等技术对催化剂物化性质进行了表征.利用固定床微型反应器评价了催化剂对甲苯和邻二甲苯完全氧化反应的催化性能.研究结果表明，采用熔融盐法制得的Co3O4具有规整八面体形貌，棱长约为300 nm.AuPd合金纳米粒子均匀分布在Co3O4表面，粒径为2.7-3.2 nm.在所得催化剂中，0.96（AuPd1.92）/Co3O4催化剂对甲苯和邻二甲苯完全氧化反应表现出较高的催化活性.在空速为40000 mL/（g·h）时，甲苯和邻二甲苯转化率达到90%所需的温度分别为180和187℃.我们认为0.96（AuPd1.92）/Co3O4催化剂较为优异的催化性能与AuPd纳米粒子和Co3O4之间的强相互作用和较高的吸附氧浓度有关.

关键词: 熔融盐, 四氧化三钴, AuPd纳米粒子, 挥发性有机物, 催化氧化

Abstract:

Using the molten salt and polyvinyl alcohol-protected reduction method, we fabricated Co3O4 octahedron-supported Au-Pd (x(AuPdy)/Co3O4; x=(0.18, 0.47, and 0.96) wt%; y (Pd/Au molar ratio)=1.85-1.97) nanocatalysts. The molten salt-derived Co3O4 sample possessed well-defined octahedral morphology, with an edge length of 300 nm. The Au-Pd nanoparticles, with sizes of 2.7-3.2 nm, were uniformly dispersed on the surface of Co3O4. The 0.96(AuPd1.92)/Co3O4 sample showed the highest catalytic activity for toluene and o-xylene oxidation, and the temperature required for achieving 90% conversion of toluene and o-xylene was 180 and 187℃, respectively, at a space velocity of 40000 mL/(g·h). The high catalytic performance of Co3O4 octahedron-supported Au-Pd nanocatalysts was associated with the interaction between Au-Pd nanoparticles and Co3O4 and high concentration of adsorbed oxygen species.

Key words: Molten salt, Cobalt oxide, Au-Pd nanoparticle, Volatile organic compound, Catalytic oxidation