Au-Pd/3DOM Co3O4: Highly active and stable nanocatalysts for toluene oxidation

Au-Pd/3DOM Co3O4: Highly active and stable nanocatalysts for toluene oxidation
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Au-Pd/3DOM Co3O4:高活性、稳定的甲苯氧化纳米催化剂

DOI:
10.1016/j.jcat.2014.09.024
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发表时间:
2015-02-01
影响因子:
7.3
通讯作者:
Dai, Hongxing
Dai, Hongxing
中科院分区:
化学1区
文献类型:
--
作者:
Xie, Shaohua;Deng, Jiguang;Dai, Hongxing

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采用聚甲基丙烯酸甲酯模板法和聚乙烯醇保护还原法制备了三维有序大孔(3DOM)Co 3 O 4及其负载的金钯合金(xAuPd/3DOM Co 3 O 4,x = 0.50-1.99 wt%,Au/Pd质量比= 1:1)纳米催化剂。3DOM Co 3 O 4负载的Au-Pd样品的性能比负载的单一Au或Pd样品好得多,其中1.99 AuPd/3DOM Co 3 O 4样品显示出最佳性能:T-10%、T-50%和T-90%(实现甲苯转化率10%、50%和90%所需的温度)在空速40,000 mL/(g h)下为145、164和168摄氏度,分别3DOMCo 3 O 4负载Au-Pd纳米催化剂对甲苯的氧化反应也表现出比负载Au或Pd样品更好的催化稳定性和更强的耐湿能力。xAuPd/3DOMCo 3 O 4催化剂的表观活化能(33-41 kJ/mol)远低于3DOMCo 3 O 4和负载单一Au或Pd样品的表观活化能(52-112 kJ/mol),其中1.99AuPd/3DOMCo 3 O 4催化剂的表观活化能最低(33 kJ/mol)。结果表明,1.99AuPd/3DOMCo 3 O 4催化剂具有较好的氧活化能力和较强的贵金属-3DOMCo 3 O 4相互作用是其优异催化性能的主要原因。(C)2014 Elsevier Inc. All rights reserved.
The polymethyl methacrylate-templating and polyvinyl alcohol-protected reduction routes were adopted to prepared three-dimensionally ordered macroporous (3DOM) Co3O4 and its supported gold-palladium alloy (xAuPd/3DOM Co3O4, x = 0.50-1.99 wt% and Au/Pd mass ratio = 1:1) nanocatalysts. The 3DOM Co3O4 supported Au-Pd samples performed much better than supported single Au or Pd samples, with the 1.99AuPd/3DOM Co304 sample showing the best performance: the T-10%, T-50%, and T-90% (temperatures required for achieving toluene conversions of 10%, 50%, and 90%) were 145, 164, and 168 degrees C at a space velocity of 40,000 mL/(g h), respectively. The 3DOM Co3O4 supported Au-Pd nanocatalysts also exhibited better catalytic stability and more moisture-tolerant ability than the supported Au or Pd samples for toluene oxidation. The apparent activation energies (33-41 kJ/mol) over xAuPd/3DOM Co3O4 were much lower than those (52-112 kJ/mol) over 3DOM Co3O4 and supported single Au or Pd samples, with the 1.99AuPd/3DOM Co3O4 sample exhibiting the lowest apparent activation energy (33 kJ/mol). It is concluded that better oxygen activation ability and stronger noble metal-3DOM Co3O4 interaction were responsible for the excellent catalytic performance of 1.99AuPd/3DOM Co3O4. (C) 2014 Elsevier Inc. All rights reserved.