化工进展 ›› 2019, Vol. 38 ›› Issue (9): 4102-4108.DOI: 10.16085/j.issn.1000-6613.2018-2218

• 工业催化 • 上一篇    下一篇

Ru-CeO x /TiO2复合氧化物催化HCl氧化反应制Cl2

石坚(),惠丰,袁俊,梅苏宁,余秦伟,张前,王为强,李亚妮,赵锋伟,杨建明(),吕剑()   

  1. 西安近代化学研究所,氟氮化工资源高效开发与利用国家重点实验室,陕西 西安710065
  • 收稿日期:2018-11-14 出版日期:2019-09-05 发布日期:2019-09-05
  • 通讯作者: 杨建明,吕剑
  • 作者简介:石坚(1994—),男,硕士研究生,研究方向为工业催化。E-mail:a38860075@126.com
  • 基金资助:
    陕西省科技创新统筹创新工程计划(2017ZDXM-GY-073)

Ru-CeO x /TiO2 composite oxide for catalytic oxidation of HCl to Cl2

Jian SHI(),Feng HUI,Jun YUAN,Suning MEI,Qinwei YU,Qian ZHANG,Weiqiang WANG,Yani LI,Fengwei ZHAO,Jianming YANG(),Jian LÜ()   

  1. State Key Laboratory of Fluorine & Nitrogen Chemicals, Xi’an Modern Chemistry Research Institute, Xi’an 710065, Shaanxi, China
  • Received:2018-11-14 Online:2019-09-05 Published:2019-09-05
  • Contact: Jianming YANG,Jian Lü

摘要:

为提高钌基催化剂的高温稳定性,本文采用液相共浸法制备了一系列Ru-CeO x /TiO2复合氧化物催化剂,探究了CeO2对钌基催化剂在HCl氧化过程中催化性能的影响。通过TEM、XRD、N2吸附-脱附、Raman、XPS等表征手段分析催化剂结构及组成,结合催化剂在HCl催化氧化反应中的催化性能,研究了不同Ce负载量对RuO2/TiO2体系的作用规律。结果表明,引入Ce之后改变了活性相RuO2与载体TiO2的相互作用,形成了Ce-O-Ru结构,对钌基催化剂的活性产生一定的负面作用;但是由于抑制了Ru活性位点的烧结失活,同时高浓度的Ce3+物种有利于氧物种的吸附与活化,使含适量Ce的Ru-CeO x /TiO2复合氧化物催化剂能够在较高温度(370℃、400℃)下保持良好的高温稳定性与催化活性,最终确定摩尔比以Ru∶Ce=1∶1较为适宜。

关键词: Ru-CeO x /TiO2复合氧化物, 氯化氢, 氯气, 催化, 氧化, 稳定性

Abstract:

To improve the stability of Ru-based catalyst under high temperature, a series of Ru-CeO x /TiO2 composite oxide catalysts were prepared by a liquid co-impregnation method. The influence of CeO2 on the Ru-based catalysts for catalytic oxidation of HCl was investigated. The catalysts with different loading amount of Ce were characterized by TEM, XRD, N2 adsorption-desorption, Raman and XPS, and the results were correlated with the catalytic performance. The results indicated that the introduction of Ce changed the interactions of the active phase of RuO2 and the support TiO2, and the formation of Ce-O-Ru structure decreased the catalytic activity. Nevertheless, the sintering of Ru active sites was suppressed and a high concentration of Ce3+ was generated which was favorable for the adsorption and activation of oxygen species. Finally, the Ru-CeO x /TiO2 composite oxide catalysts with a proper amount of Ce gave an excellent high-temperature stability and activity, and the appropriate mole ratio of Ru to Ce was 1.0.

Key words: Ru-CeO x /TiO2 composite oxide, chlorine hydride, chlorine, catalysis, oxidation, stability

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