Qiqi Shi , Yujing Zhang , Xiao Zhang , Boxiong Shen , Kai Ren , Hanming Wu
{"title":"介孔锰-钴-钛对邻二甲苯降解的催化性能:实际条件下的机理研究","authors":"Qiqi Shi , Yujing Zhang , Xiao Zhang , Boxiong Shen , Kai Ren , Hanming Wu","doi":"10.1016/j.fuproc.2023.108021","DOIUrl":null,"url":null,"abstract":"<div><p>Catalytic combustion of volatile organic compounds from industrial flue gases at low temperatures remains a challenge. Herein, we developed a mesoporous Mn-Co-Ti catalyst for o-xylene degradation by a solvothermal strategy. The optimized Mn<sub>0.1</sub>Co-TiO<sub>2</sub> catalyst possessed a nanoflower structures with a surface area of 83.1 m<sup>2</sup>/g and mesoporous volume of 0.1191 cm<sup>3</sup>/g. Mn-doping modulated the electronic interactions between Mn and Co, which promoted the formation of MnCo<sub>2</sub>O<sub>4.5</sub> phase and increased Co<sup>3+</sup> and Mn<sup>4+</sup> content of the catalyst. The Mn<sub>0.1</sub>Co-TiO<sub>2</sub> catalyst had an improved reduction capacity from 170 to 644 °C, with a maximum H<sub>2</sub> consumption of 4.56 mmol/g. The Mn<sub>0.1</sub>Co-TiO<sub>2</sub> catalyst achieved 50% o-xylene conversion at 193 °C at a GHSV of 60,000 h<sup>−1</sup>, whereas the equivalent catalyst prepared by impregnation required 315 °C for 50% o-xylene conversion. In the presence of NO, the generated NO<sub>2</sub> accelerated o-xylene conversion because it promoted the generation of more Mn<sup>4+</sup>-O-Co<sup>3+</sup> active sites and accumulation of intermediates such as maleate and acetate species. NH<sub>3</sub> and H<sub>2</sub>O had slight inhibitory effects on o-xylene conversion, which were attenuated by abundant mesopores and redox ability of catalyst. SO<sub>2</sub> gas caused inactive sulfates and chemical deactivation on catalyst surface, thus leading to excessive formation of benzoquinone products.</p></div>","PeriodicalId":326,"journal":{"name":"Fuel Processing Technology","volume":"253 ","pages":"Article 108021"},"PeriodicalIF":7.2000,"publicationDate":"2023-12-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S0378382023003697/pdfft?md5=26abad710ef9281622a5377d63a1e771&pid=1-s2.0-S0378382023003697-main.pdf","citationCount":"0","resultStr":"{\"title\":\"Catalytic performance of mesoporous Mn-Co-Ti for o-xylene degradation: Mechanistic study under practical conditions\",\"authors\":\"Qiqi Shi , Yujing Zhang , Xiao Zhang , Boxiong Shen , Kai Ren , Hanming Wu\",\"doi\":\"10.1016/j.fuproc.2023.108021\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Catalytic combustion of volatile organic compounds from industrial flue gases at low temperatures remains a challenge. Herein, we developed a mesoporous Mn-Co-Ti catalyst for o-xylene degradation by a solvothermal strategy. The optimized Mn<sub>0.1</sub>Co-TiO<sub>2</sub> catalyst possessed a nanoflower structures with a surface area of 83.1 m<sup>2</sup>/g and mesoporous volume of 0.1191 cm<sup>3</sup>/g. Mn-doping modulated the electronic interactions between Mn and Co, which promoted the formation of MnCo<sub>2</sub>O<sub>4.5</sub> phase and increased Co<sup>3+</sup> and Mn<sup>4+</sup> content of the catalyst. The Mn<sub>0.1</sub>Co-TiO<sub>2</sub> catalyst had an improved reduction capacity from 170 to 644 °C, with a maximum H<sub>2</sub> consumption of 4.56 mmol/g. The Mn<sub>0.1</sub>Co-TiO<sub>2</sub> catalyst achieved 50% o-xylene conversion at 193 °C at a GHSV of 60,000 h<sup>−1</sup>, whereas the equivalent catalyst prepared by impregnation required 315 °C for 50% o-xylene conversion. In the presence of NO, the generated NO<sub>2</sub> accelerated o-xylene conversion because it promoted the generation of more Mn<sup>4+</sup>-O-Co<sup>3+</sup> active sites and accumulation of intermediates such as maleate and acetate species. NH<sub>3</sub> and H<sub>2</sub>O had slight inhibitory effects on o-xylene conversion, which were attenuated by abundant mesopores and redox ability of catalyst. SO<sub>2</sub> gas caused inactive sulfates and chemical deactivation on catalyst surface, thus leading to excessive formation of benzoquinone products.</p></div>\",\"PeriodicalId\":326,\"journal\":{\"name\":\"Fuel Processing Technology\",\"volume\":\"253 \",\"pages\":\"Article 108021\"},\"PeriodicalIF\":7.2000,\"publicationDate\":\"2023-12-26\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://www.sciencedirect.com/science/article/pii/S0378382023003697/pdfft?md5=26abad710ef9281622a5377d63a1e771&pid=1-s2.0-S0378382023003697-main.pdf\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Fuel Processing Technology\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0378382023003697\",\"RegionNum\":2,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, APPLIED\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Fuel Processing Technology","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0378382023003697","RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, APPLIED","Score":null,"Total":0}
Catalytic performance of mesoporous Mn-Co-Ti for o-xylene degradation: Mechanistic study under practical conditions
Catalytic combustion of volatile organic compounds from industrial flue gases at low temperatures remains a challenge. Herein, we developed a mesoporous Mn-Co-Ti catalyst for o-xylene degradation by a solvothermal strategy. The optimized Mn0.1Co-TiO2 catalyst possessed a nanoflower structures with a surface area of 83.1 m2/g and mesoporous volume of 0.1191 cm3/g. Mn-doping modulated the electronic interactions between Mn and Co, which promoted the formation of MnCo2O4.5 phase and increased Co3+ and Mn4+ content of the catalyst. The Mn0.1Co-TiO2 catalyst had an improved reduction capacity from 170 to 644 °C, with a maximum H2 consumption of 4.56 mmol/g. The Mn0.1Co-TiO2 catalyst achieved 50% o-xylene conversion at 193 °C at a GHSV of 60,000 h−1, whereas the equivalent catalyst prepared by impregnation required 315 °C for 50% o-xylene conversion. In the presence of NO, the generated NO2 accelerated o-xylene conversion because it promoted the generation of more Mn4+-O-Co3+ active sites and accumulation of intermediates such as maleate and acetate species. NH3 and H2O had slight inhibitory effects on o-xylene conversion, which were attenuated by abundant mesopores and redox ability of catalyst. SO2 gas caused inactive sulfates and chemical deactivation on catalyst surface, thus leading to excessive formation of benzoquinone products.
期刊介绍:
Fuel Processing Technology (FPT) deals with the scientific and technological aspects of converting fossil and renewable resources to clean fuels, value-added chemicals, fuel-related advanced carbon materials and by-products. In addition to the traditional non-nuclear fossil fuels, biomass and wastes, papers on the integration of renewables such as solar and wind energy and energy storage into the fuel processing processes, as well as papers on the production and conversion of non-carbon-containing fuels such as hydrogen and ammonia, are also welcome. While chemical conversion is emphasized, papers on advanced physical conversion processes are also considered for publication in FPT. Papers on the fundamental aspects of fuel structure and properties will also be considered.