Aiyong Wang*, Min Ding, Yuang Cai, Li Wang, Yun Guo, Yanglong Guo and Wangcheng Zhan*,
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引用次数: 0
摘要
CeO2 极易受到氯中毒的影响,导致其效率和稳定性降低,从而阻碍了在 CeO2 上氧化氯化挥发性有机化合物。本研究设计了 Ru 和 Nb 共修饰的 CeO2 催化剂,在催化氧化 1,2-二氯乙烷 (EDC) 的过程中实现了优异的活性、稳定性和二氧化碳选择性。据观察,Nb-O-Ce 键的形成增强了表面酸性位点,从而提高了盐酸选择性并减少了氯化副产物的产生。同时,它抑制了 Ru-O-Ce 的形成,促进了表面高度分散的 RuO2 颗粒的生成,增强了表面氧的氧化还原特性和流动性,从而提高了 CO2 的选择性。原位漫反射红外傅立叶变换光谱结果表明,氯物种优先附着在 Ru/Nb/CeO2 催化剂上的 Nb 物种上,而不是氧空位上。这使得更多的烷烃基团在氧空位上氧化成甲酸酯,从而降低了副产物浓度。此外,在 RuO2 的协同作用下,烷基开始氧化成羧酸,完成了一个全面的氧化过程。
Ultra-efficient Ru and Nb Co-Modified CeO2 Catalysts for Catalytic Oxidation of 1,2-Dichloroethane
The oxidation of chlorinated volatile organic compounds on CeO2 is hindered by its high susceptibility to chlorine poisoning, resulting in a reduced efficiency and stability. In this study, Ru- and Nb-co-modified CeO2 catalysts were designed to achieve excellent activity, stability, and CO2 selectivity in the catalytic oxidation of 1,2-dichloroethane (EDC). The formation of Nb–O–Ce bonds was observed to enhance the surface acidic sites, thereby improving HCl selectivity and reducing the production of chlorinated byproducts. Meanwhile, it inhibits the formation of Ru–O–Ce and promotes the generation of highly dispersed RuO2 particles on the surface, enhancing the redox properties and mobility of the surface oxygen, thus increasing CO2 selectivity. In situ diffuse reflectance infrared Fourier transform spectroscopy results revealed that chlorine species preferentially attach to Nb species rather than to oxygen vacancies on the Ru/Nb/CeO2 catalyst. This allows more alkane groups to oxidize to formate on the oxygen vacancies, reducing byproduct concentration. Additionally, the oxidation of alkane groups to carboxylic acids is initiated on the Nb species, completing a comprehensive oxidation process under the synergistic effect of RuO2.
期刊介绍:
Environmental Science & Technology (ES&T) is a co-sponsored academic and technical magazine by the Hubei Provincial Environmental Protection Bureau and the Hubei Provincial Academy of Environmental Sciences.
Environmental Science & Technology (ES&T) holds the status of Chinese core journals, scientific papers source journals of China, Chinese Science Citation Database source journals, and Chinese Academic Journal Comprehensive Evaluation Database source journals. This publication focuses on the academic field of environmental protection, featuring articles related to environmental protection and technical advancements.