石油炼制与化工 ›› 2025, Vol. 56 ›› Issue (3): 18-26.

• 催化剂 • 上一篇    下一篇

ConCu1Ox@NF催化剂的制备及其催化甲苯氧化性能

刘文举,潘达,袁凯龙,张政,侯亚芳,冯秋悦,党丹,王少锋   

  1. 河南工业大学化学化工学院
  • 收稿日期:2024-10-09 修回日期:2024-11-20 出版日期:2025-03-12 发布日期:2025-02-25
  • 通讯作者: 刘文举 E-mail:wenjuliu@haut.edu.cn
  • 基金资助:
    河南省自然科学基金项目

PREPARATION OF ConCu1Ox@NF CATALYSTS AND THEIR CATALYTIC PERFORMANCE FOR TOLUENE OXIDATION

#br#   


  • Received:2024-10-09 Revised:2024-11-20 Online:2025-03-12 Published:2025-02-25

摘要: 以泡沫镍(NF)为载体,采用原位电沉积法制备了不同Co/Cu物质的量比的整体式催化氧化催化剂ConCu1Ox@NF(n为Co/Cu物质的量比,n为0.5,1,2,3)。其中,在原料甲苯质量浓度为1 000 mg/m3、空速为15 000 mL/(g.h)的条件下,Co3Cu1Ox@NF催化甲苯氧化降解的性能最佳,其T20(达到20%转化率时所对应的温度)和T90(达到90%转化率时所对应的温度)分别为201 ℃和219 ℃。此外,Co3Cu1Ox@NF催化甲苯氧化的表观活化能最小(21.79 kJ/mol),且其在40 h的稳定性测试中,催化活性并没有出现下降,具有优异的稳定性。通过一系列表征手段探究Co3Cu1Ox@NF催化性能优异的原因,结果表明,Co3Cu1Ox@NF催化剂表面具有三维网状结构,活性物质已成功负载且分散均匀,具有最高的Co3+/Co2+物质的量比和Oads/OLatt物质的量比,丰富的氧缺陷和优异的氧化还原性能。

关键词: 催化氧化, 整体式催化剂, 甲苯, 泡沫镍, 电沉积法

Abstract: A series of monolithic catalysts ConCu1Ox@NF(n = 0.5, 1, 2, 3)with varying Co/Cu molar ratios were synthesised via in situ electrodeposition using nickel foam as carrier. The catalyst Co3Cu1Ox@NF demonstrated the most effective catalytic activity for the catalytic oxidation of toluene, with T20 and T90 values of 201℃ and 219℃, respectively, at a concentration of toluene of 1 000 mg/m3 and a space velocity of 15 000 mL/(g.h). Furthermore, the catalyst Co3Cu1Ox@NF exhibited the lowest apparent activation energy for the catalytic oxidation of toluene(Ea = 21.79 kJ/mol), the catalytic activity remained stable throughout the 40 h stability test, exhibiting excellent stability. The physicochemical properties of the catalysts were investigated using SEM, EDS, XRD, XPS, Raman spectroscopy and H2-TPR. The results demonstrate that the Co3Cu1Ox@NF catalyst surface exhibits a three-dimensional mesh structure, with the active substances successfully loaded and uniformly dispersed. Additionally, the Co3+/Co2+ and Oads/OLatt ratios are at their highest, and the oxygen defects and redox properties are abundant and excellent.

Key words: catalytic oxidation, monolithic catalyst, toluene, nickel foam, electrodeposition