Insight into the promotion effect of H2O for the simultaneous removal of NOx and methanol at low temperature over MnFe2Ox catalyst

IF 7.2 2区 工程技术 Q1 ENGINEERING, CHEMICAL Journal of Environmental Chemical Engineering Pub Date : 2025-06-01 Epub Date: 2025-03-10 DOI:10.1016/j.jece.2025.116113
Yunli Ji, Xuanyi Wen, Wenbo Geng, Xia An, Xu Wu
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Abstract

The research on the simultaneous removal of NOx and VOCs by NH3-SCR catalysts has garnered widespread attention. However, the stepwise removal of both gases during the co-removal process is often caused by the inconsistent activity windows. Furthermore, the presence of water vapor in flue gas adversely impacts the catalyst and greatly decreases its catalytic activity. In this study, the low-temperature catalyst MnFe2Ox was selected to remove NOx and methanol, with a focus on investigating the influence of H2O on catalytic reactions. Results show that MnFe2Ox exhibited nearly 100 % denitrification activity and methanol oxidation performance within 150–240 °C. H2O in the atmosphere scarcely affected the performance of the synergistic removal and positively influenced N2 generation. Catalyst characterizations conducted with or without H2O demonstrated that nitrogen-containing gases were inhibited from adhering to the catalyst surface by the competitive adsorption of H2O. Furthermore, the dehydrogenation of NH3 active species to -NH2/-NH was impeded, which reduced the likelihood of unintended reactions that generate N2O. The DRIFTs analysis of the simultaneous removal reaction indicates that the presence of H2O facilitates the formation of significant intermediates like methyl nitrite and isocyanate from methanol, which could hydrolyze to produce NH3, CO and other reducing gases that would react with NOx to maintain NOx removal efficiency. These results offer direction for further research into the influence of water vapor in flue gas on the co-removal of NOx and VOCs.
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H2O对mnfe2o催化剂上低温同时脱除NOx和甲醇的促进作用
NH3-SCR催化剂同时去除NOx和VOCs的研究受到了广泛关注。然而,在共去除过程中,两种气体的逐步去除通常是由不一致的活动窗口引起的。此外,烟气中水蒸气的存在对催化剂产生不利影响,大大降低了催化剂的催化活性。本研究选择低温催化剂mnfe2o去除NOx和甲醇,重点研究H2O对催化反应的影响。结果表明,在150 ~ 240℃范围内,mnfeox具有接近100% %的脱氮活性和甲醇氧化性能。大气中H2O对协同去除效果影响不大,对N2生成有积极影响。在有水或没有水的情况下进行的催化剂表征表明,由于水的竞争性吸附,含氮气体被抑制在催化剂表面上。此外,NH3活性物质脱氢成-NH2/ -NH2受到阻碍,这降低了产生N2O的意外反应的可能性。同时脱除反应的DRIFTs分析表明,H2O的存在有利于甲醇生成亚硝酸盐甲酯、异氰酸酯等重要中间体,这些中间体可以水解生成NH3、CO等还原性气体,这些还原性气体与NOx发生反应,维持NOx的脱除效率。这些结果为进一步研究烟气中水蒸气对NOx和VOCs协同去除的影响提供了方向。
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来源期刊
Journal of Environmental Chemical Engineering
Journal of Environmental Chemical Engineering Environmental Science-Pollution
CiteScore
11.40
自引率
6.50%
发文量
2017
审稿时长
27 days
期刊介绍: The Journal of Environmental Chemical Engineering (JECE) serves as a platform for the dissemination of original and innovative research focusing on the advancement of environmentally-friendly, sustainable technologies. JECE emphasizes the transition towards a carbon-neutral circular economy and a self-sufficient bio-based economy. Topics covered include soil, water, wastewater, and air decontamination; pollution monitoring, prevention, and control; advanced analytics, sensors, impact and risk assessment methodologies in environmental chemical engineering; resource recovery (water, nutrients, materials, energy); industrial ecology; valorization of waste streams; waste management (including e-waste); climate-water-energy-food nexus; novel materials for environmental, chemical, and energy applications; sustainability and environmental safety; water digitalization, water data science, and machine learning; process integration and intensification; recent developments in green chemistry for synthesis, catalysis, and energy; and original research on contaminants of emerging concern, persistent chemicals, and priority substances, including microplastics, nanoplastics, nanomaterials, micropollutants, antimicrobial resistance genes, and emerging pathogens (viruses, bacteria, parasites) of environmental significance.
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