含硫气氛中Ce改性Cu-Mn/Al_(2)O_(3)低温催化氧化CO性能研究  

Low-temperature catalytic CO oxidation performance of Ce-modified Cu-Mn/Al_(2)O_(3) in sulfur-containing atmospheres

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作  者:王正芳 高君安 张傑[1] 曲令多 WANG ZhengFang;GAO JunAn;ZHANG Jie;QU LingDuo(College of Chemical Engineering,Beijing University of Chemical Technology,Beijing 100029;Zibo Qichuang New Material Technology Co.Ltd.,Zibo 255100,China)

机构地区:[1]北京化工大学化学工程学院,北京100029 [2]淄博齐创新材料科技有限公司,淄博255100

出  处:《北京化工大学学报(自然科学版)》2024年第3期22-33,共12页Journal of Beijing University of Chemical Technology(Natural Science Edition)

基  金:国家重点研发计划(2021YFF0307401)。

摘  要:为了解决Cu-Mn催化剂在含硫气氛中催化氧化CO时快速失活的问题,以Cu-Mn为活性组分、Ce改性的γ-Al_(2)O_(3)为载体制备了Ce改性Cu-Mn/Al_(2)O_(3)催化剂,并采用扫描电子显微镜(SEM)、X射线衍射(XRD)、N2吸附-脱附测试(BET)、氢气程序升温还原(H_(2)-TPR)、X射线光电子能谱(XPS)对其进行了表征,结果表明:CeO_(2)的加入提高了活性组分的分散度,降低了Cu-Mn/Al_(2)O_(3)催化剂的还原温度,增加了Cu^(2+)、Mn^(3+)及氧空位的含量。测试了Ce改性Cu-Mn/Al_(2)O_(3)催化剂的CO催化氧化活性及抗硫中毒性能,发现Ce的加入可以提高催化剂的CO催化氧化性能,采用浸渍法改性(Ce)/Al_(2)O_(3)载体(Ce负载量为2%)制备的催化剂(10Cu_(1)Mn_(2)/2(Ce)/Al_(2)O_(3))的催化性能较高,可以在130℃下实现CO完全氧化;添加Ce后催化剂的抗硫中毒性能有一定提升,在160℃下通入SO_(2)后5 h,催化剂10Cu_(1)Mn_(2)/2(Ce)/Al_(2)O_(3)能够维持57%左右的CO转化率,在300℃下测试25 h该催化剂的活性没有下降。In order to solve the problem of rapid deactivation of Cu-Mn catalysts in the catalytic oxidation of CO in sulfur-containing atmospheres,a Ce-modified Cu-Mn/Al_(2)O_(3)catalyst was prepared by using Cu-Mn as the active component,and Ce-modifiedγ-Al_(2)O_(3)as the support.The catalyst was characterized by scanning electron microscopy(SEM),X-ray diffraction(XRD),N_(2)adsorption-desorption measurements(BET),hydrogen temperature programmed reduction(H2-TPR)and X-ray photoelectron spectroscopy(XPS).The results show that the addition of CeO_(2)can improve the dispersion of active components,reduce the reduction temperature of the Cu-Mn/Al_(2)O_(3)catalyst,and increase the content of Cu^(2+),Mn^(3+)and oxygen vacancies.The CO catalytic oxidation activity and sulfur poisoning resistance of the Ce-modified Cu-Mn/Al_(2)O_(3)catalyst were tested.It was found that the addition of Ce improved the CO catalytic oxidation performance of the catalyst.The catalyst 10Cu_(1)Mn_(2)/2(Ce)/Al_(2)O_(3)prepared using a(Ce)/Al_(2)O_(3)support(with a Ce loading of 2%)modified using an impregnation method had higher catalytic performance and could achieve complete oxidation of CO at 130℃.The sulfur poisoning resistance of the catalyst was enhanced after the addition of Ce.After the introduction of SO_(2)at 160℃for 5 h,the catalyst 10Cu_(1)Mn_(2)/2(Ce)/Al_(2)O_(3)maintained a CO conversion of about 57%.Furthermore,the activity of the catalyst did not decrease even after 25 h at 300℃.

关 键 词:CeO_(2) Cu-Mn/Al_(2)O_(3) CO催化氧化 抗硫中毒 

分 类 号:TQ426.8[化学工程]

 

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