Relationship between Physicochemical Properties and Toluene Oxidation Performance of the CeOx–CrOx Catalysts

IF 3 3区 化学 Q2 CHEMISTRY, APPLIED
Dong Ye, Xiaoxiang Wang, Kai Zhu, Ke Wu
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引用次数: 0

Abstract

A series of CeOx–CrOx catalysts were synthesized via the sol-gel method for the oxidation of toluene. A comprehensive set of characterization techniques, including XRD, N2 adsorption, Raman spectroscopy, HRTEM, H2-TPR, O2-TPD, XPS, and in situ DRIFTS, was employed to investigate the structure-performance relationships of the catalysts. Among the catalysts, the one with a Ce/Cr molar ratio of 1:3 exhibited the best performance in toluene oxidation, with the activation energy for toluene degradation decreasing from 54.5 kJ mol−1 for CeOx to 31.3 kJ mol−1 for the CeOx–CrOx (1:3) and CO2 selectivity reaching 100% at temperatures above 250 °C. This enhancement was primarily attributed to an increased specific surface area, an elevated concentration of highly active Cr6+ species, and improved reducibility and mobility of surface oxygen species. During the reaction, toluene was rapidly adsorbed and converted into benzoate intermediates, which were subsequently oxidized to form the final products, CO2 and H2O.

Abstract Image

CeOx-CrOx催化剂的理化性质与甲苯氧化性能的关系
采用溶胶-凝胶法合成了一系列用于甲苯氧化的CeOx-CrOx催化剂。采用XRD、N2吸附、拉曼光谱、HRTEM、H2-TPR、O2-TPD、XPS、原位漂移等综合表征技术对催化剂的结构性能关系进行了研究。其中,Ce/Cr摩尔比为1:3的催化剂对甲苯的氧化性能最好,对甲苯的降解活化能从CeOx的54.5 kJ mol−1降至CeOx - crox的31.3 kJ mol−1(1:3),在250℃以上的温度下,CO2选择性达到100%。这种增强主要归因于比表面积的增加,高活性Cr6+物质浓度的提高,以及表面氧的还原性和迁移性的改善。在反应过程中,甲苯被快速吸附并转化为苯甲酸酯中间体,随后被氧化生成最终产物CO2和H2O。
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来源期刊
Topics in Catalysis
Topics in Catalysis 化学-物理化学
CiteScore
5.70
自引率
5.60%
发文量
197
审稿时长
2 months
期刊介绍: Topics in Catalysis publishes topical collections in all fields of catalysis which are composed only of invited articles from leading authors. The journal documents today’s emerging and critical trends in all branches of catalysis. Each themed issue is organized by renowned Guest Editors in collaboration with the Editors-in-Chief. Proposals for new topics are welcome and should be submitted directly to the Editors-in-Chief. The publication of individual uninvited original research articles can be sent to our sister journal Catalysis Letters. This journal aims for rapid publication of high-impact original research articles in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis.
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