富氧空位ε-氧化锰/氧化锰钒复合催化剂对甲醛去除效果的评价

IF 20.2 1区 化学 Q1 CHEMISTRY, PHYSICAL Applied Catalysis B: Environmental Pub Date : 2023-01-01 DOI:10.1016/j.apcatb.2022.121994
Xuan Liu , Jialin Wu , Shuai Zhang , Qiang Li , Zhaojun Wu , Jianbin Zhang
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引用次数: 9

摘要

除甲醛对健康至关重要,但构建高性能非贵金属催化剂仍面临巨大挑战,其中通过掺杂改性增加氧空位是提高催化活性的先进策略。本文基于热分解策略合成了一种具有协同效应的ε-MnO2/Mn2V2O7复合催化剂。同时,在不添加模板剂和表面活性剂的情况下,由co2储存材料、Mn2+和钒酸盐反应合成了催化剂的前驱体。在催化剂的辅助下,20 mg/L的10 mL甲醛(HCHO)溶液在30℃下循环5次,1h后降解率可达72.0%,并维持在67%以上。随后,所获得的协同催化机理表明,高价V5+可能部分取代MnO2框架中的Mn4+,通过Mn4+/Mn3+和V5+/V4+的氧化还原偶联,促进复合催化剂表面形成富氧空位(V4+-□-Mn3+)。这导致了吸附氧的增加,显著提高了HCHO的降解性能。本研究为开发优质非贵金属催化剂的掺杂改性提供了一种新颖而先进的方法。
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Evaluation of an ε-manganese (IV) oxide/manganese vanadium oxide composite catalyst enriched with oxygen vacancies for enhanced formaldehyde removal

Formaldehyde removal is vital to health, but the construction of high-performance non-precious metal catalysts still faces great challenges, in which increasing oxygen vacancies by dopant modification is an advanced strategy to enhance catalytic activity. In this work, a novel ε-MnO2/Mn2V2O7 composite catalyst with a synergistic effect was synthesized on the basis of a thermal decomposition strategy. Meanwhile, the precursor for the catalyst was synthesized from the reaction among CO2-storage material, Mn2+, and vanadate without additional template agents and surfactants. Aided by the catalyst, the degradation rate of a 20 mg/L 10 mL formaldehyde (HCHO) solution can reach 72.0% and maintain above 67% after 5 cycles at 30 °C for 1 h. Subsequently, the as-obtained synergistic catalytic mechanism showed that the high-valent V5+ may partially replace Mn4+ in the MnO2 framework, promoting the formation of enriched oxygen vacancies (V4+-□-Mn3+) on the surface of the composite catalyst via the redox coupling of Mn4+/Mn3+ and V5+/V4+. This leads to an increase in adsorbed oxygen, significantly improving the degradation performance of HCHO. This work provides a novel and advanced strategy for dopant modification to develop superior non-precious metal catalysts.

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来源期刊
Applied Catalysis B: Environmental
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.
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