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CeO2-WO3催化剂表面酸性和氧化还原性能在脱硝反应中的研究

康海彦 莫杜娟 张学军 张梦茹 高洪润 毛艳丽 李海洋 宋忠贤

康海彦, 莫杜娟, 张学军, 张梦茹, 高洪润, 毛艳丽, 李海洋, 宋忠贤. CeO2-WO3催化剂表面酸性和氧化还原性能在脱硝反应中的研究[J]. 燃料化学学报(中英文), 2023, 51(6): 812-822. doi: 10.19906/j.cnki.JFCT.2023005
引用本文: 康海彦, 莫杜娟, 张学军, 张梦茹, 高洪润, 毛艳丽, 李海洋, 宋忠贤. CeO2-WO3催化剂表面酸性和氧化还原性能在脱硝反应中的研究[J]. 燃料化学学报(中英文), 2023, 51(6): 812-822. doi: 10.19906/j.cnki.JFCT.2023005
KANG Hai-yan, MO Du-juan, ZHANG Xue-jun, ZHANG Meng-ru, GAO Hong-run, MAO Yan-li, LI Hai-yang, SONG Zhong-xian. Investigation of the surface acidity and redox on the CeO2-WO3 catalyst for selective catalytic reduction with NH3[J]. Journal of Fuel Chemistry and Technology, 2023, 51(6): 812-822. doi: 10.19906/j.cnki.JFCT.2023005
Citation: KANG Hai-yan, MO Du-juan, ZHANG Xue-jun, ZHANG Meng-ru, GAO Hong-run, MAO Yan-li, LI Hai-yang, SONG Zhong-xian. Investigation of the surface acidity and redox on the CeO2-WO3 catalyst for selective catalytic reduction with NH3[J]. Journal of Fuel Chemistry and Technology, 2023, 51(6): 812-822. doi: 10.19906/j.cnki.JFCT.2023005

CeO2-WO3催化剂表面酸性和氧化还原性能在脱硝反应中的研究

doi: 10.19906/j.cnki.JFCT.2023005
基金项目: 国家自然科学基金(21872096),河南省青年自然科学基金(202300410034),河南城建学院骨干教师项目(YCJQNGGJS201903),河南城建学院学术带头人项目(YCJXSJSDTR202204),平顶山市2021年重大科技专项(2021ZD03)和河南城建学院博士启动基金(990/Q2017011)资助
详细信息
    通讯作者:

    E-mail: xjzhang_syict@163.com

    songzhongxian@126.com

  • 中图分类号: O643

Investigation of the surface acidity and redox on the CeO2-WO3 catalyst for selective catalytic reduction with NH3

Funds: The project was supported by the National Natural Science Foundation of China (21872096), Natural Science Youth Fund of Henan Province (202300410034), Young Teacher Foundation of Henan University of Urban Construction (YCJQNGGJS201903), Academic Leader of Henan Institute of Urban Construction (YCJXSJSDTR202204), Science and technology major special of Pingdingshan (2021ZD03) and Doctoral Research Start-up Project of Henan University of Urban Construction (990/Q2017011)
  • 摘要: 本研究利用原位合成法成功制备CeO2-WO3催化剂并用于脱硝反应,焙烧温度为550 ℃的CW-550催化剂活性最佳,200 ℃时CW-550脱硝活性达到90%以上。CW-550催化剂具有优越的催化剂性能可归结为较大的比表面积、较多的Ce3 + 物种、丰富的表面酸性和优越的氧化还原性能。Ce3 + 增多,有利于氧空位的形成,可促进氧化还原性能。WO3的引入,在550 ℃的焙烧条件下可显著提升催化剂的Brönsted酸量,有利于氨气的吸附与活化,提升其催化性能。CW催化剂上吸附的NH3物种能与气态的NO反应,而吸附态的NH3与吸附态的NOx不能进行高效反应,因此,CW催化剂的SCR反应主要遵循Eley-Rideal反应机理。
  • FIG. 2386.  FIG. 2386.

    FIG. 2386.  FIG. 2386.

    图  1  CW催化剂的NOx转化率(a), NO2生成量(b), N2O浓度和N2选择性(c)和XRD谱图

    Figure  1  (a) Catalyst CW of NOx conversion, (b) NO2 production, (c) N2O concentration and N2 selectivity, (d) XRD patterns of catalyst CW

    图  2  (a) CW催化剂N2吸附-脱附等温线,(b) 孔径分布,(c) 拉曼光谱谱图,(d) H2-TPR谱图

    Figure  2  (a) Catalyst CW of N2 adsorption-desorption isotherms, (b) pore size distribution, (c) Raman spectra, (d) H2-TPR

    图  3  CW催化剂在200 ℃下NH3吸附原位漫反射红外光谱谱图

    Figure  3  In-situ DRIFTS spectra of CW catalyst adsorbed NH3 at 200 ℃

    (a): CW-450; (b): CW-500; (c): CW-550; (d): CW-600

    图  4  CW催化剂在200 ℃下吸附NO + O2的原位漫反射红外光谱谱图

    Figure  4  In-situ DRIFTS spectea of CW catalyst adsorbed NO + O2 at 200 ℃

    (a): CW-450; (b): CW-500; (c): CW-550; (d): CW-600

    图  5  预吸附NH3与NO + O2反应的原位漫反射红外光谱谱图

    Figure  5  In-situ DRIFTS spectra of reaction between NO + O2 and pre-adsorption NH3 species over (e): CW-450; (f): CW-500; (g): CW-550

    图  6  预吸附NO + O2和NH3反应的原位漫反射红外光谱谱图

    Figure  6  In-situ DRIFTS spectra of reaction between NH3 and pre-adsorption NO + O2 species over

    (a): CW-450; (b): CW-500; (c): CW-550; (d): CW-600

    图  7  CW催化剂SCR反应途径示意图

    Figure  7  SCR reaction pathway of CW catalyst

    表  1  表面原子比

    Table  1  Surface atom concentration (%)

    SampleCe3 + /(Ce4 + + Ce3 + )Oα/(Oα + Oβ)
    CW-45020.6425.76
    CW-50021.4233.30
    CW-55023.9416.81
    CW-60023.0826.85
    下载: 导出CSV
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  • 收稿日期:  2022-08-21
  • 修回日期:  2022-10-09
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