Synergistic mechanism of hetero-interfacial oxygen vacancies on catalytic oxidation of 1,2-dichloroethane over Ru-modified monolayer-dispersed WOx/CeO2 catalysts: Differences in distribution of active sites

IF 20.2 1区化学 Q1 CHEMISTRY, PHYSICAL

Applied Catalysis B: Environmental Pub Date : 2023-12-25 DOI:10.1016/j.apcatb.2023.123664

Xinyu Meng , Qirui Wang , Wei Wang , Tiantian Zhang , Yan Sun , Yuliang Shi , Shuiliang Yao , Zuliang Wu , Jing Li , Erhao Gao , Jiali Zhu , Qiguang Dai

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Abstract

Ru-modified monolayer-dispersed WO_x/CeO₂ hybrid composites were prepared by co-impregnation (CI) and step impregnation (SI) methods, and the effects of active site distribution on the catalytic oxidation of 1,2-dichloroethane (DCE) were investigated. Ru species tends to be deposited on the monolayer-dispersed WO_x (m-WO_x) by SI method, which can increase the oxygen vacancies (O_V,m-WOx) at m-WO_x/CeO₂ interfaces. Abundant O_V,m-WOx can promote the formation of more active W–OH and accelerate the dechloridation and oxydehydrogenation of DCE. Oppositely, for CI method, Ru species exists mainly in the form of Ru−O−Ce bonds, increasing the oxygen vacancies (O_V,RuCe) into CeO₂ surface lattices and promoting the deep oxidation of intermediate products. The closer contact between the two hetero-interfacial oxygen vacancies (O_V,RuCe and O_V,m-WOx) on Ru-modified m-WO_x/CeO₂ produces a stronger synergistic effect on DCE activation and oxidation, and meanwhile advantageously inhibits the adsorption of chlorine species as well as the formation of polychlorinated by-products.

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异质界面氧空位在 Ru 改性单层分散 WOx/CeO2 催化剂上催化氧化 1,2-二氯乙烷的协同机制：活性位点分布的差异

采用共浸渍法（CI）和阶跃浸渍法（SI）制备了Ru修饰的单层分散WOx/CeO2杂化复合材料，研究了活性位点分布对1,2-二氯乙烷（DCE）催化氧化的影响。通过 SI 法，Ru 物种倾向于沉积在单层分散的 WOx（m-WOx）上，从而增加了 m-WOx/CeO2 界面的氧空位（OV,m-WOx）。丰富的 OV,m-WOx 可促进形成更多的活性 W-OH，并加速 DCE 的脱氯和氧脱氢反应。相反，在 CI 法中，Ru 物种主要以 Ru-O-Ce 键的形式存在，增加了 CeO2 表面晶格中的氧空位（OV,RuCe），促进了中间产物的深度氧化。在 Ru 改性的 m-WOx/CeO2 上，两个异质界面氧空位（OV,RuCe 和 OV,m-WOx）之间的接触更加紧密，对二氯乙烯的活化和氧化产生了更强的协同效应，同时有利地抑制了氯物种的吸附以及多氯副产物的形成。

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来源期刊

Applied Catalysis B: Environmental 环境科学-工程：化工

CiteScore

38.60

自引率

6.30%

发文量

1117

审稿时长

24 days

期刊介绍： Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including: 1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources. 2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes. 3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts. 4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells. 5.Catalytic reactions that convert wastes into useful products. 6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts. 7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems. 8.New catalytic combustion technologies and catalysts. 9.New catalytic non-enzymatic transformations of biomass components. The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.