化学工程2024,Vol.52Issue(10) :19-24,38.DOI:10.3969/j.issn.1005-9954.2024.10.004

Cu-TiO2@CeO2催化剂催化氧化NH3/Hg0

Catalytic oxidation of NH3/Hg0 by Cu-TiO2@CeO2 catalyst

陈传敏 彭钦磊 曹悦 吴佳艺 陈韵伊 刘妍 刘松涛 贾文波
化学工程2024,Vol.52Issue(10) :19-24,38.DOI:10.3969/j.issn.1005-9954.2024.10.004

Cu-TiO2@CeO2催化剂催化氧化NH3/Hg0

Catalytic oxidation of NH3/Hg0 by Cu-TiO2@CeO2 catalyst

陈传敏 1彭钦磊 1曹悦 1吴佳艺 2陈韵伊 2刘妍 2刘松涛 1贾文波1
扫码查看

作者信息

  • 1. 华北电力大学环境科学与工程系,河北保定 071003;华北电力大学区域能源系统优化教育部重点实验室,北京 102206
  • 2. 华北电力大学环境科学与工程系,河北保定 071003
  • 折叠

摘要

为了减少SCR系统逃逸氨和气态单质汞的排放,采用模板法制备一系列具有氨氧化和汞氧化活性的Cu-TiO2@CeO2催化剂,在150-400℃下测试其氨氧化和汞氧化性能,并对其进行了 XRD(X射线衍射)、BET(比表面积测试)和XPS(X射线光电子能谱)表征.结果表明:高温可以促进NH3的氧化,但不利于保持高N2选择性和Hg0氧化效果.随着铜、铈质量分数的增加,催化剂的氨氧化和汞氧化活性均逐渐增加,而N2选择性有所下降.其中Cu、Ce质量分数为5%的Cu-TiO2@CeO2-5催化剂可以达到较为理想的NH3和Hg0去除效果,350℃下对NH3和Hg0的氧化效率均高于90%,N2选择性在95%以上,副产物N2O生成量低于5 ×10-6.表征结果显示Cu-TiO2@CeO2催化剂中形成了 Cu++Ce4+⇌Cu2++Ce3+氧化还原双电对,Cu与Ce的氧化物在NH3和Hg0氧化反应中起协同作用,大量的Oβ作为活性氧参与到反应中,有效促进了 NH3和Hg0的催化脱除.

Abstract

In order to mitigate the release of escaping ammonia and gaseous elemental mercury in the SCR system,a series of Cu-TiO2@CeO2 catalysts with mercury and ammoxidation activities were synthesized using the template method.The ammoxidation and mercury oxidation properties were evaluated at 150-400 ℃,and the catalysts were characterized by XRD,BET and XPS.The results indicate that high temperature can enhance the oxidation of NH3 but is not favorable for maintaining high N2 selectivity and Hg0 oxidation performance.With the increase of the mass fractions of Cu and Ce,the activities of ammonia oxidation and mercury oxidation of the catalyst gradually increase,but the selectivity of N2 decreases.Among them,Cu-TiO2@CeO2-5 catalyst with 5%mass fractions of Cu and Ce can achieve ideal removal of NH3 and Hg0.At 350 ℃,the oxidation efficiencies of NH3 and Hg0 are both above 90%,the N2 selectivity is above 95%,and the by-product N2O formation is below 5 × 10-6.The characterization results show that Cu++Ce4+⇌Cu2++Ce3+redox double electric pair forms in the catalyst.The oxides of Cu and Ce act synergically in the oxidation reaction of NH3 and Hg0.A large amount of Oβ participate in the reaction as active oxygen species,effectively promoting the catalytic removal of NH3 and Hg0 concentrations.

关键词

///氨氧化/双功能催化剂/核壳结构

Key words

copper/cerium/mercury/ammonia oxidation/bifunctional catalyst/core-shell structure

引用本文复制引用

基金项目

国家自然科学基金资助项目(52300129)

中央高校基本科研专项资金资助项目(2022MS103)

大学生创新创业项目(S202310079142)

出版年

2024
化学工程
华陆工程科技有限责任公司

化学工程

CSTPCD北大核心
影响因子:0.438
ISSN:1005-9954
段落导航相关论文