{"title":"粉煤灰基ZSM-5沸石的两步水热合成及其对NO的催化性能","authors":"Jing Li , Suxia Ma , Nuo Xu","doi":"10.1016/j.jwpe.2024.106608","DOIUrl":null,"url":null,"abstract":"<div><div>The pursuit of carbon peaking and carbon neutrality goals necessitates flexible operation and deep peaking of coal-fired units, thus placing heightened demands on nitrogen oxide (NO<sub>X</sub>) emission control. Fly ash, a solid waste rich in silicon (Si) and aluminum (Al), should be fully leveraged, and the high-value synthesis of zeolite represents a viable utilization method. In this context, fly ash-based zeolite was prepared as a catalyst to facilitate the generation of active oxides from H<sub>2</sub>O<sub>2</sub>, combined with alkali solution absorption, to achieve efficient denitrification. This approach effectively transforms ‘waste to pollution’ mitigation. The optimal synthesis conditions for FA-ZSM-5 zeolite were established using the alkali fusion hydrothermal synthesis method, with fly ash as the raw material. The specified conditions were NaOH/FA = 1.2, SiO<sub>2</sub>/Al<sub>2</sub>O<sub>3</sub> = 40, H<sub>2</sub>O/Al<sub>2</sub>O<sub>3</sub> = 1325, TPAOH/Al<sub>2</sub>O<sub>3</sub> = 10, ZSM-5-seed addition of 5 %, and a hydrothermal temperature and time of 140 °C for 24 h. Experimental parameters were meticulously investigated to ascertain their impact on nitric oxide (NO) removal efficiency. The highest removal efficiency was achieved under specific conditions: a reaction temperature of 140 °C, an H<sub>2</sub>O<sub>2</sub> concentration of 6 %, a catalyst dose of 0.3 g, an NO concentration of 600 mg/m<sup>3</sup>, and an SO<sub>2</sub> concentration of 1000 mg/m<sup>3</sup>. Finally, analysis of the catalytic oxidation mechanism revealed that H<sub>2</sub>O<sub>2</sub>, when catalyzed by FA-ZSM-5 zeolite, generates ·OH radicals with strong oxidizing properties, thereby facilitating the oxidative removal of NO.</div></div>","PeriodicalId":17528,"journal":{"name":"Journal of water process engineering","volume":"69 ","pages":"Article 106608"},"PeriodicalIF":6.3000,"publicationDate":"2024-11-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"A two-step hydrothermal synthesis of fly-ash-based ZSM-5 zeolite and its catalytic properties in NO removal\",\"authors\":\"Jing Li , Suxia Ma , Nuo Xu\",\"doi\":\"10.1016/j.jwpe.2024.106608\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>The pursuit of carbon peaking and carbon neutrality goals necessitates flexible operation and deep peaking of coal-fired units, thus placing heightened demands on nitrogen oxide (NO<sub>X</sub>) emission control. Fly ash, a solid waste rich in silicon (Si) and aluminum (Al), should be fully leveraged, and the high-value synthesis of zeolite represents a viable utilization method. In this context, fly ash-based zeolite was prepared as a catalyst to facilitate the generation of active oxides from H<sub>2</sub>O<sub>2</sub>, combined with alkali solution absorption, to achieve efficient denitrification. This approach effectively transforms ‘waste to pollution’ mitigation. The optimal synthesis conditions for FA-ZSM-5 zeolite were established using the alkali fusion hydrothermal synthesis method, with fly ash as the raw material. The specified conditions were NaOH/FA = 1.2, SiO<sub>2</sub>/Al<sub>2</sub>O<sub>3</sub> = 40, H<sub>2</sub>O/Al<sub>2</sub>O<sub>3</sub> = 1325, TPAOH/Al<sub>2</sub>O<sub>3</sub> = 10, ZSM-5-seed addition of 5 %, and a hydrothermal temperature and time of 140 °C for 24 h. Experimental parameters were meticulously investigated to ascertain their impact on nitric oxide (NO) removal efficiency. The highest removal efficiency was achieved under specific conditions: a reaction temperature of 140 °C, an H<sub>2</sub>O<sub>2</sub> concentration of 6 %, a catalyst dose of 0.3 g, an NO concentration of 600 mg/m<sup>3</sup>, and an SO<sub>2</sub> concentration of 1000 mg/m<sup>3</sup>. Finally, analysis of the catalytic oxidation mechanism revealed that H<sub>2</sub>O<sub>2</sub>, when catalyzed by FA-ZSM-5 zeolite, generates ·OH radicals with strong oxidizing properties, thereby facilitating the oxidative removal of NO.</div></div>\",\"PeriodicalId\":17528,\"journal\":{\"name\":\"Journal of water process engineering\",\"volume\":\"69 \",\"pages\":\"Article 106608\"},\"PeriodicalIF\":6.3000,\"publicationDate\":\"2024-11-30\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of water process engineering\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2214714424018403\",\"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}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of water process engineering","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2214714424018403","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}
A two-step hydrothermal synthesis of fly-ash-based ZSM-5 zeolite and its catalytic properties in NO removal
The pursuit of carbon peaking and carbon neutrality goals necessitates flexible operation and deep peaking of coal-fired units, thus placing heightened demands on nitrogen oxide (NOX) emission control. Fly ash, a solid waste rich in silicon (Si) and aluminum (Al), should be fully leveraged, and the high-value synthesis of zeolite represents a viable utilization method. In this context, fly ash-based zeolite was prepared as a catalyst to facilitate the generation of active oxides from H2O2, combined with alkali solution absorption, to achieve efficient denitrification. This approach effectively transforms ‘waste to pollution’ mitigation. The optimal synthesis conditions for FA-ZSM-5 zeolite were established using the alkali fusion hydrothermal synthesis method, with fly ash as the raw material. The specified conditions were NaOH/FA = 1.2, SiO2/Al2O3 = 40, H2O/Al2O3 = 1325, TPAOH/Al2O3 = 10, ZSM-5-seed addition of 5 %, and a hydrothermal temperature and time of 140 °C for 24 h. Experimental parameters were meticulously investigated to ascertain their impact on nitric oxide (NO) removal efficiency. The highest removal efficiency was achieved under specific conditions: a reaction temperature of 140 °C, an H2O2 concentration of 6 %, a catalyst dose of 0.3 g, an NO concentration of 600 mg/m3, and an SO2 concentration of 1000 mg/m3. Finally, analysis of the catalytic oxidation mechanism revealed that H2O2, when catalyzed by FA-ZSM-5 zeolite, generates ·OH radicals with strong oxidizing properties, thereby facilitating the oxidative removal of NO.
期刊介绍:
The Journal of Water Process Engineering aims to publish refereed, high-quality research papers with significant novelty and impact in all areas of the engineering of water and wastewater processing . Papers on advanced and novel treatment processes and technologies are particularly welcome. The Journal considers papers in areas such as nanotechnology and biotechnology applications in water, novel oxidation and separation processes, membrane processes (except those for desalination) , catalytic processes for the removal of water contaminants, sustainable processes, water reuse and recycling, water use and wastewater minimization, integrated/hybrid technology, process modeling of water treatment and novel treatment processes. Submissions on the subject of adsorbents, including standard measurements of adsorption kinetics and equilibrium will only be considered if there is a genuine case for novelty and contribution, for example highly novel, sustainable adsorbents and their use: papers on activated carbon-type materials derived from natural matter, or surfactant-modified clays and related minerals, would not fulfil this criterion. The Journal particularly welcomes contributions involving environmentally, economically and socially sustainable technology for water treatment, including those which are energy-efficient, with minimal or no chemical consumption, and capable of water recycling and reuse that minimizes the direct disposal of wastewater to the aquatic environment. Papers that describe novel ideas for solving issues related to water quality and availability are also welcome, as are those that show the transfer of techniques from other disciplines. The Journal will consider papers dealing with processes for various water matrices including drinking water (except desalination), domestic, urban and industrial wastewaters, in addition to their residues. It is expected that the journal will be of particular relevance to chemical and process engineers working in the field. The Journal welcomes Full Text papers, Short Communications, State-of-the-Art Reviews and Letters to Editors and Case Studies