不同配体Ce-MOFs衍生的CeO2催化剂的制备及催化性能研究

郜晨旭, 魏伟东, 罗涛, 李换英, 白书立*

化工新型材料 ›› 2024, Vol. 52 ›› Issue (2) : 195 -200.

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化工新型材料 ›› 2024, Vol. 52 ›› Issue (2) : 195-200. DOI: 10.19817/j.cnki.issn1006-3536.2024.02.005
科学研究

不同配体Ce-MOFs衍生的CeO2催化剂的制备及催化性能研究

    郜晨旭, 魏伟东, 罗涛, 李换英, 白书立*
作者信息 +

Preparation and catalytic performance of CeO2 catalysts derived from Ce-MOFs with different ligands

  • Gao Chenxu, Wei Weidong, Luo Tao, Li Huanying, Bai Shuli
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摘要

通过水热合成法合成了有机配体不同的前驱体铈基金属-有机骨架,经过400℃煅烧得到CeO2催化剂用于催化氧化甲苯,并研究了催化剂的性能。结果表明,在反应温度为180~260℃、质量空速为60000mL/(g·h)条件下,催化剂活性顺序为CeO2-B>CeO2-M>CeO2-A(B、M、A分别是有机配体4,4′-联吡啶、2-甲基咪唑、2-氨基对苯二甲酸的英文首字母)。CeO2-B在215℃对甲苯的降解率达到92.9%,在30h稳定性测试中保持优异的催化性能,其优异的催化活性得益于较大的比表面积(126.72m2/g)、孔容(0.19cm3/g)、平均孔径(5.44nm)、较高的Ce3+含量(19.97%)和表面化学吸附氧含量(43.63%)。X射线衍射、全自动比表面积分析仪、扫描电子显微镜、氢气-程序升温还原、X射线光电子能谱等表征证明,有机配体会影响催化剂的比表面积、孔容、孔径和粒径等物理性质。

Abstract

The cerium-metal-organic frameworks (Ce-MOFs),a precursor with different organic ligands,was synthesized by hydrothermal synthesis,and the CeO2 catalysts for catalytic oxidation of toluene were obtained by calcination at 400℃,and the properties of the catalyst were studied.The results showed that under the conditions of the reaction temperature of 180~260℃and the mass airspeed of 60000mL/(g·h),the order of activity of the catalysts was:CeO2-B>CeO2-M>CeO2-A(B,M and A were the initials of organic ligands 4,4′-bipyridine,2-methylimidazole,and 2-aminoterephthalic acid,respectively).CeO2-B achieved a toluene degradation rate of 92.9% at 215℃and maintained excellent catalytic performance in the 30h stability test.Its outstanding catalytic activity benefited from the large specific surface area (126.72m2/g),pore volume (0.19cm3/g),average pore size (5.44nm),the higher concentrations of Ce3+ (19.97%) and surface chemisorption oxygen Oads(43.63%).XRD,BET,SEM,H2-TPR,XPS and other characterizations proved that organic ligands affected the physical properties of catalysts such as specific surface area,pore volume,pore size and particle size.

关键词

金属-有机骨架(MOFs) / 氧化铈 / 有机配体 / 催化性能 / 甲苯

Key words

MOFs / CeO2 / organic ligands / catalytic performance / toluene

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不同配体Ce-MOFs衍生的CeO2催化剂的制备及催化性能研究[J]. 化工新型材料, 2024, 52(2): 195-200 DOI:10.19817/j.cnki.issn1006-3536.2024.02.005

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基金资助

国家自然科学基金(21006065)

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