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LaFeO3钙钛矿催化湿式氧化苯酚的研究

刘鑫尧 张宣娇 杨淑倩 韩蛟 李印福 张磊 高志贤

刘鑫尧, 张宣娇, 杨淑倩, 韩蛟, 李印福, 张磊, 高志贤. LaFeO3钙钛矿催化湿式氧化苯酚的研究[J]. 燃料化学学报. doi: 10.19906/j.cnki.JFCT.2022044
引用本文: 刘鑫尧, 张宣娇, 杨淑倩, 韩蛟, 李印福, 张磊, 高志贤. LaFeO3钙钛矿催化湿式氧化苯酚的研究[J]. 燃料化学学报. doi: 10.19906/j.cnki.JFCT.2022044
LIU Xin-yao, ZHANG Xuan-jiao, YANG Shu-qian, HAN Jiao, LI Yin-fu, ZHANG Lei, GAO Zhi-xian. Study on Wet Air Oxidation of Phenol catalyzed by LaFeO3 perovskite[J]. Journal of Fuel Chemistry and Technology. doi: 10.19906/j.cnki.JFCT.2022044
Citation: LIU Xin-yao, ZHANG Xuan-jiao, YANG Shu-qian, HAN Jiao, LI Yin-fu, ZHANG Lei, GAO Zhi-xian. Study on Wet Air Oxidation of Phenol catalyzed by LaFeO3 perovskite[J]. Journal of Fuel Chemistry and Technology. doi: 10.19906/j.cnki.JFCT.2022044

LaFeO3钙钛矿催化湿式氧化苯酚的研究

doi: 10.19906/j.cnki.JFCT.2022044
基金项目: 国家自然科学基金(21673270)和辽宁省教育厅科学研究经费项目(L2019012)资助
详细信息
    通讯作者:

    张磊(1983—),男,副教授,lnpuzhanglei@163.com

    高志贤(1964—),男,教授,gaozx@lnpu.edu.cn

  • 中图分类号: O643

Study on Wet Air Oxidation of Phenol catalyzed by LaFeO3 perovskite

Funds: The project was supported by the National Natural Science Foundation of China (21673270);The Scientific Research Funds project of Education Department of Liaoning Province (L2019012)
  • 摘要: 本研究采用固相球磨法制备了四种不同球磨时间的LaFeO3钙钛矿催化材料,并将其用于催化湿式氧化苯酚反应,探讨了球磨时间对LaFeO3钙钛矿催化剂催化湿式氧化苯酚水溶液性能的影响。采用XRD、H2-TPR、TG-DTA、FT-IR、N2物理吸附、XPS等手段对LaFeO3钙钛矿催化材料进行了表征。结果表明,在反应温度为200 ℃、空气压力5 MPa、苯酚初始浓度4000 mg/L时,经过240 min的催化氧化反应后LaFeO3-6催化材料最终的COD去除率为94.5%。
  • 图  1  不同球磨时间的XRD谱图

    Figure  1  XRD patterns of different milling time

    a: LaFeO3-4; b: LaFeO3-6; c: LaFeO3-8; d: LaFeO3-10

    图  2  LaFeO3-t的FT-IR谱图

    Figure  2  FT-IR patterns of the LaFeO3-t catalysts

    a: LaFeO3-4; b: LaFeO3-6; c: LaFeO3-8; d: LaFeO3-10

    图  3  LaFeO3-t催化材料的N2吸附-脱附等温线

    Figure  3  N2 Adsorption and desorption isotherms of N2 from LaFeO3-t catalytic materials

    a: LaFeO3-4; b: LaFeO3-6; c: LaFeO3-8; d: LaFeO3-10

    图  4  LaFeO3-t催化材料的H2-TPR谱图

    Figure  4  TPR profiles of catalysts LaFeO3-t

    a: LaFeO3-4; b: LaFeO3-6; c: LaFeO3-8; d: LaFeO3-10

    图  5  LaFeO3前驱体的TG-DTA曲线

    Figure  5  TG-DTA curves of LaFeO3 precursor

    图  6  LaFeO3-t催化剂中La 3d的XPS谱图

    Figure  6  XPS spectra of La 3d prepared by LaFeO3-t

    a: LaFeO3-4; b: LaFeO3-6; c: LaFeO3-8; d: LaFeO3-10

    图  7  LaFeO3-t催化剂中Fe 2p的XPS谱图

    Figure  7  XPS Spectra of Fe 2p of LaFeO3-t Catalyst

    a: LaFeO3-4; b: LaFeO3-6; c: LaFeO3-8; d: LaFeO3-10

    图  8  LaFeO3-t钙钛矿催化剂中O 1s 的XPS 谱图

    Figure  8  XPS spectra of O 1s prepared by LaFeO3-t perovskite catalysts

    a: LaFeO3-4; b: LaFeO3-6; c: LaFeO3-8; d: LaFeO3-10

    图  9  LaFeO3-t钙钛矿复合金属氧化物催化湿式氧化苯酚性能

    Figure  9  CWAO of phenol over the LaFeO3-t catalysts

    表  1  LaFeO3-t的结构参数表

    Table  1  Structural parameters of LaFeO3-t

    CatalystLaFeO3−4LaFeO3−6LaFeO3−8LaFeO3−10
    Specific surface area /(m2·g−1) 15.8 18.2 14.7 14.7
    Pore volume /(cm3·g−1) 0.10 0.08 0.08 0.09
    Average crystallite size /nm 20.7 18.9 20.0 20.9
    下载: 导出CSV

    表  2  LaFeO3-t催化材料的还原峰位置

    Table  2  Reduction of LaFeO3-t catalyst

    CatalystPeak temperature t/℃
    α peakβ peakγ peak
    LaFeO3-4 371 467 673
    LaFeO3-6 333 436 601
    LaFeO3-8 351 448 616
    LaFeO3-10 353 451 636
    下载: 导出CSV

    表  3  LaFeO3-t催化剂中O 1s XPS曲线拟合

    Table  3  O 1s XPS curve-fitting results of LaFeO3-t catalysts

    CatalystOads/(Oads+OLa–O–CO3+Olatt)(%)
    LaFeO3-437.4
    LaFeO3-640.6
    LaFeO3-840.3
    LaFeO3-1039.5
    下载: 导出CSV

    表  4  催化材料的重复使用性

    Table  4  The repetition of the catalyst

    Reuse times1234
    COD removal rate/%94.591.788.285.8
    下载: 导出CSV
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  • 收稿日期:  2022-03-21
  • 录用日期:  2022-05-05
  • 修回日期:  2022-05-02
  • 网络出版日期:  2022-06-09

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