{"title":"Insight into the promotion effect of H2O for the simultaneous removal of NOx and methanol at low temperature over MnFe2Ox catalyst","authors":"Yunli Ji, Xuanyi Wen, Wenbo Geng, Xia An, Xu Wu","doi":"10.1016/j.jece.2025.116113","DOIUrl":null,"url":null,"abstract":"<div><div>The research on the simultaneous removal of NO<sub>x</sub> and VOCs by NH<sub>3</sub>-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 MnFe<sub>2</sub>O<sub>x</sub> was selected to remove NO<sub>x</sub> and methanol, with a focus on investigating the influence of H<sub>2</sub>O on catalytic reactions. Results show that MnFe<sub>2</sub>O<sub>x</sub> exhibited nearly 100 % denitrification activity and methanol oxidation performance within 150–240 °C. H<sub>2</sub>O in the atmosphere scarcely affected the performance of the synergistic removal and positively influenced N<sub>2</sub> generation. Catalyst characterizations conducted with or without H<sub>2</sub>O demonstrated that nitrogen-containing gases were inhibited from adhering to the catalyst surface by the competitive adsorption of H<sub>2</sub>O. Furthermore, the dehydrogenation of NH<sub>3</sub> active species to -NH<sub>2</sub>/-NH was impeded, which reduced the likelihood of unintended reactions that generate N<sub>2</sub>O. The DRIFTs analysis of the simultaneous removal reaction indicates that the presence of H<sub>2</sub>O facilitates the formation of significant intermediates like methyl nitrite and isocyanate from methanol, which could hydrolyze to produce NH<sub>3</sub>, CO and other reducing gases that would react with NO<sub>x</sub> to maintain NO<sub>x</sub> removal efficiency. These results offer direction for further research into the influence of water vapor in flue gas on the co-removal of NO<sub>x</sub> and VOCs.</div></div>","PeriodicalId":15759,"journal":{"name":"Journal of Environmental Chemical Engineering","volume":"13 3","pages":"Article 116113"},"PeriodicalIF":7.4000,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Environmental Chemical Engineering","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2213343725008097","RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
引用次数: 0
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.
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.