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双金属Cu-Ce/SAPO-34催化剂的制备及其NH3-SCR脱硝性能研究

刘崇飞 王学涛 邢利利 程星星 张兴宇 丁坤

刘崇飞, 王学涛, 邢利利, 程星星, 张兴宇, 丁坤. 双金属Cu-Ce/SAPO-34催化剂的制备及其NH3-SCR脱硝性能研究[J]. 燃料化学学报. doi: 10.19906/j.cnki.JFCT.2022034
引用本文: 刘崇飞, 王学涛, 邢利利, 程星星, 张兴宇, 丁坤. 双金属Cu-Ce/SAPO-34催化剂的制备及其NH3-SCR脱硝性能研究[J]. 燃料化学学报. doi: 10.19906/j.cnki.JFCT.2022034
LIU Chong-fei, WANG Xue-tao, XING Li-li, CHENG Xing-xing, ZHANG Xing-yu, DING Kun. Study on Preparation and denitrification performance of NH3-SCR of bimetallic Cu-Ce/SAPO-34 catalyst[J]. Journal of Fuel Chemistry and Technology. doi: 10.19906/j.cnki.JFCT.2022034
Citation: LIU Chong-fei, WANG Xue-tao, XING Li-li, CHENG Xing-xing, ZHANG Xing-yu, DING Kun. Study on Preparation and denitrification performance of NH3-SCR of bimetallic Cu-Ce/SAPO-34 catalyst[J]. Journal of Fuel Chemistry and Technology. doi: 10.19906/j.cnki.JFCT.2022034

双金属Cu-Ce/SAPO-34催化剂的制备及其NH3-SCR脱硝性能研究

doi: 10.19906/j.cnki.JFCT.2022034
基金项目: 国家自然科学基金(50806020),河南省科技创新人才计划(杰出青年)(114100510010)和河南省科技攻关项目(152102210280)资助
详细信息
    作者简介:

    刘崇飞(1994-),男,河南洛阳人,河南科技大学硕士生,主要从事清洁高效燃烧、废弃物能源化利用等方面的研究。E-mail: 2803541886@qq.com

    通讯作者:

    E-mail: wxt7682@163.com

  • 中图分类号: TK229.6;X701;X511

Study on Preparation and denitrification performance of NH3-SCR of bimetallic Cu-Ce/SAPO-34 catalyst

Funds: Project Supported by National Natural Science Foundation of China (50806020); Henan Science and Technology Innovation Talent Program (Outstanding Youth) (114100510010); Science and Technology Project of Science and Technology Department of Henan Province(152102210280).
More Information
  • 摘要: 采用浸渍法制备了Cu-Ce双金属系列分子筛催化剂(Cu-Ce/SAPO-34),在催化剂评价装置上考察了不同质量比Cu/Ce的分子筛催化剂选择性催化还原NO的性能。通过XRD、SEM、NH3-TPD、XPS、in-situ DRIFTS等多种表征手段对催化剂的结构及微观特性进行了分析。结果表明,改性后Cu-Ce/SAPO-34催化剂脱硝性能良好,具有较宽的活性温度窗口,当Cu、Ce的含量均为4%时,分子筛催化剂脱硝效率最好,在325−500℃脱硝效率均在80%,在400−500 ℃时,脱硝效率达到了99%以上。双金属Cu-Ce氧化物物种高度分散于催化剂表面,SAPO-34的晶体结构未受影响,且活性物质和载体之间产生较好的相互作用。4Cu-4Ce/SAPO-34具有适量的酸性位点,该配比对催化剂的脱硝性能和稳定性具有积极作用,在NH3-SCR反应过程中遵循E-R机理。
  • 图  1  不同Cu/Ce质量比催化剂的脱硝效率

    Figure  1  NO conversion of catalysts with different Cu/Ce mass ratios

    图  2  不同Cu/Ce质量比催化剂的XRD谱图

    Figure  2  XRD patterns of catalysts with different Cu/Ce mass ratios

    图  3  不同Cu/Ce质量比催化剂的SEM图像(倍数分别为10000、1000倍)

    Figure  3  SEM images of different Cu/Ce mass ratios(the multiples are 10000 and 1000 respectively)

    图  4  不同Cu/Ce质量比催化剂的NH3-TPD谱图

    Figure  4  NH3-TPD spectra of catalysts with different Cu / Ce mass ratios

    图  5  不同催化剂的XPS谱图

    Figure  5  XPS profiles of different catalysts

    图  6  4Cu-4Ce/SAPO-34催化剂表面NH3吸附in-situ DRIFTS谱图

    Figure  6  In-situ DRIFTS of NH3 adsorbed over the 4Cu-4Ce/SAPO-34 catalyst

    图  7  4Cu-4Ce/SAPO-34催化剂表面NH3吸附饱和后通入NO+O2 in-situ DRIFTS谱图

    Figure  7  In-situ DRIFTS of NO+O2 reacting with pre-adsorbed NH3 over the 4Cu-4Ce/SAPO-34 catalyst

    图  8  4Cu-4Ce/SAPO-34催化剂表面NO+O2吸附in-situ DRIFTS谱图

    Figure  8  In-situ DRIFTS of NO+O2 adsorbed over the 4Cu-4Ce/SAPO-34 catalyst

    图  9  4Cu-4Ce/SAPO-34催化剂表面NO+O2吸附饱和后通入NH3 in-situ DRIFTS谱图

    Figure  9  In-situ DRIFTS of NH3 reacting with pre-adsorbed NO+O2 over the 4Cu-4Ce/SAPO-34 catalyst

    表  1  不同价态金属离子的特征峰面积

    Table  1  Characteristic peak areas of metal ions with different valence states

    CatalystCu+Cu2+Ce3+Ce4+
    4Cu/SAPO-347966.64387.3
    4Cu-4Ce/SAPO-345345.67127.310575341376.7
    4Ce/SAPO-3491606.251107.9
    下载: 导出CSV
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  • 收稿日期:  2022-02-09
  • 录用日期:  2022-04-14
  • 修回日期:  2022-04-14
  • 网络出版日期:  2022-04-29

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