{"title":"异相Fe-Ce@SiC/H2O2体系的构建及其对NO的去除","authors":"Wenxia Zhao , Zehao Zhou , Xiaomeng Guo , Zhongyang Wang , Yicong Yu , Xin Wang , Dingchao Zhang , Yanhu Zhang","doi":"10.1016/j.apcata.2025.120374","DOIUrl":null,"url":null,"abstract":"<div><div>Conventional SCR denitrification technology often encounters difficulties in adapting to the flue gas scenarios characterized by low temperatures and high moisture. Therefore developing a low-temperature denitrification process that is both cost-effective and efficient is crucial. In this paper, a heterogeneous Fe-Ce@SiC/H<sub>2</sub>O<sub>2</sub> oxidation-absorption system was constructed. The NO removal performances of this system were systematically investigated. The results show that, compared with the acidic conditions, the heterogeneous Fe-Ce@SiC/H<sub>2</sub>O<sub>2</sub> system under the alkaline conditions exhibited better NO removal performance. Specifically, under optimal experimental conditions, the removal efficiency of NO in the Fe-Ce@SiC/H<sub>2</sub>O<sub>2</sub> system could reach up to 87.1 %. When the circulating water flow rate was further increased to 600 ml/min, NO could be completely removed. Combined with the results of SEM, XRD, BET, XPS, EPR, the gas-liquid phase products analysis, and the radical quenching experiments, the electrochemical test, the possible reaction mechanism was proposed. The electron transfer and co-catalysis between Fe and Ce facilitated the regeneration of the metal active sites, therefore, H<sub>2</sub>O<sub>2</sub> was enhanced to produce more •O<sub>2</sub><sup>-</sup> radicals under the catalysis of Fe-Ce@SiC. These •O<sub>2</sub><sup>-</sup> radicals are the principal active species for NO oxidation under the alkaline conditions, whereas •OH radicals and <sup>1</sup>O<sub>2</sub> are relatively less active. The purified NO is mainly converted into NO<sub>3</sub><sup>-</sup> and a small amount of NO<sub>2</sub><sup>-</sup> in the absorption solution. The research results not only further improve the theoretical system of NOx removal by the heterogeneous Fenton system, but also expand the applicability of this technology in the field of flue gas denitrification.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"704 ","pages":"Article 120374"},"PeriodicalIF":4.7000,"publicationDate":"2025-05-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Construction of heterogeneous Fe-Ce@SiC/H2O2 system and its NO removal\",\"authors\":\"Wenxia Zhao , Zehao Zhou , Xiaomeng Guo , Zhongyang Wang , Yicong Yu , Xin Wang , Dingchao Zhang , Yanhu Zhang\",\"doi\":\"10.1016/j.apcata.2025.120374\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Conventional SCR denitrification technology often encounters difficulties in adapting to the flue gas scenarios characterized by low temperatures and high moisture. Therefore developing a low-temperature denitrification process that is both cost-effective and efficient is crucial. In this paper, a heterogeneous Fe-Ce@SiC/H<sub>2</sub>O<sub>2</sub> oxidation-absorption system was constructed. The NO removal performances of this system were systematically investigated. The results show that, compared with the acidic conditions, the heterogeneous Fe-Ce@SiC/H<sub>2</sub>O<sub>2</sub> system under the alkaline conditions exhibited better NO removal performance. Specifically, under optimal experimental conditions, the removal efficiency of NO in the Fe-Ce@SiC/H<sub>2</sub>O<sub>2</sub> system could reach up to 87.1 %. When the circulating water flow rate was further increased to 600 ml/min, NO could be completely removed. Combined with the results of SEM, XRD, BET, XPS, EPR, the gas-liquid phase products analysis, and the radical quenching experiments, the electrochemical test, the possible reaction mechanism was proposed. The electron transfer and co-catalysis between Fe and Ce facilitated the regeneration of the metal active sites, therefore, H<sub>2</sub>O<sub>2</sub> was enhanced to produce more •O<sub>2</sub><sup>-</sup> radicals under the catalysis of Fe-Ce@SiC. These •O<sub>2</sub><sup>-</sup> radicals are the principal active species for NO oxidation under the alkaline conditions, whereas •OH radicals and <sup>1</sup>O<sub>2</sub> are relatively less active. The purified NO is mainly converted into NO<sub>3</sub><sup>-</sup> and a small amount of NO<sub>2</sub><sup>-</sup> in the absorption solution. The research results not only further improve the theoretical system of NOx removal by the heterogeneous Fenton system, but also expand the applicability of this technology in the field of flue gas denitrification.</div></div>\",\"PeriodicalId\":243,\"journal\":{\"name\":\"Applied Catalysis A: General\",\"volume\":\"704 \",\"pages\":\"Article 120374\"},\"PeriodicalIF\":4.7000,\"publicationDate\":\"2025-05-26\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Applied Catalysis A: General\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0926860X25002753\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Applied Catalysis A: General","FirstCategoryId":"1","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0926860X25002753","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Construction of heterogeneous Fe-Ce@SiC/H2O2 system and its NO removal
Conventional SCR denitrification technology often encounters difficulties in adapting to the flue gas scenarios characterized by low temperatures and high moisture. Therefore developing a low-temperature denitrification process that is both cost-effective and efficient is crucial. In this paper, a heterogeneous Fe-Ce@SiC/H2O2 oxidation-absorption system was constructed. The NO removal performances of this system were systematically investigated. The results show that, compared with the acidic conditions, the heterogeneous Fe-Ce@SiC/H2O2 system under the alkaline conditions exhibited better NO removal performance. Specifically, under optimal experimental conditions, the removal efficiency of NO in the Fe-Ce@SiC/H2O2 system could reach up to 87.1 %. When the circulating water flow rate was further increased to 600 ml/min, NO could be completely removed. Combined with the results of SEM, XRD, BET, XPS, EPR, the gas-liquid phase products analysis, and the radical quenching experiments, the electrochemical test, the possible reaction mechanism was proposed. The electron transfer and co-catalysis between Fe and Ce facilitated the regeneration of the metal active sites, therefore, H2O2 was enhanced to produce more •O2- radicals under the catalysis of Fe-Ce@SiC. These •O2- radicals are the principal active species for NO oxidation under the alkaline conditions, whereas •OH radicals and 1O2 are relatively less active. The purified NO is mainly converted into NO3- and a small amount of NO2- in the absorption solution. The research results not only further improve the theoretical system of NOx removal by the heterogeneous Fenton system, but also expand the applicability of this technology in the field of flue gas denitrification.
期刊介绍:
Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications.
Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.