Xin Gao , Jiaxin Song , Xiaoqiang Fan , Xuehua Yu , Lian Kong , Xia Xiao , Zean Xie , Zhen Zhao
{"title":"Ti诱导Mn2O3和Na2WO4之间的协同效应增强了甲烷在Mn2O3 - Na2WO4/TS-1催化剂上的氧化偶联","authors":"Xin Gao , Jiaxin Song , Xiaoqiang Fan , Xuehua Yu , Lian Kong , Xia Xiao , Zean Xie , Zhen Zhao","doi":"10.1039/d5cy00097a","DOIUrl":null,"url":null,"abstract":"<div><div>Oxidative coupling of methane (OCM) can directly convert natural gas into C<sub>2</sub> hydrocarbons (C<sub>2</sub>H<sub>4</sub> and C<sub>2</sub>H<sub>6</sub>). The Mn<sub>2</sub>O<sub>3</sub>–Na<sub>2</sub>WO<sub>4</sub>/SiO<sub>2</sub> catalyst, owing to its high OCM performance and thermostability at high temperatures, has become a promising OCM catalyst. The synergy and dispersion of Na<sub>2</sub>WO<sub>4</sub> and Mn<sub>2</sub>O<sub>3</sub> are important factors in improving OCM performance, and the selection of the support has a significant impact on their dispersion and interaction. To enhance the synergistic effect and dispersion of Na<sub>2</sub>WO<sub>4</sub> and Mn<sub>2</sub>O<sub>3</sub>, a TS-1 support doped with varying amounts of Ti was selected for the Mn<sub>2</sub>O<sub>3</sub>–Na<sub>2</sub>WO<sub>4</sub>/<em>x</em>TS-1 (Na–W–Mn/<em>x</em>TS-1) catalyst preparation. The characterization results showed that Ti addition promoted Na<sub>2</sub>WO<sub>4</sub> dispersion and enhanced interactions between Na<sub>2</sub>WO<sub>4</sub> and Mn<sub>2</sub>O<sub>3</sub>. Moreover, Ti doping effectively promoted the generation of active oxygen species and increased the conversion of methane, thereby increasing the C<sub>2</sub> yield. The Na–W–Mn/8%TS-1 catalyst exhibited the highest OCM performance, with a 20.0% C<sub>2</sub> yield and 46.8% CH<sub>4</sub> conversion. The enhanced OCM performance may be caused by the increased dispersion of Na<sub>2</sub>WO<sub>4</sub> and Mn<sub>2</sub>O<sub>3</sub> induced by the atomic-level Ti doping in the TS-1 support, which promoted their interaction and increased the number of lattice oxygen species.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"15 8","pages":"Pages 2628-2641"},"PeriodicalIF":4.4000,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Enhanced oxidative coupling of methane over Mn2O3–Na2WO4/TS-1 catalysts by the Ti induced synergistic effect between Mn2O3 and Na2WO4\",\"authors\":\"Xin Gao , Jiaxin Song , Xiaoqiang Fan , Xuehua Yu , Lian Kong , Xia Xiao , Zean Xie , Zhen Zhao\",\"doi\":\"10.1039/d5cy00097a\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Oxidative coupling of methane (OCM) can directly convert natural gas into C<sub>2</sub> hydrocarbons (C<sub>2</sub>H<sub>4</sub> and C<sub>2</sub>H<sub>6</sub>). The Mn<sub>2</sub>O<sub>3</sub>–Na<sub>2</sub>WO<sub>4</sub>/SiO<sub>2</sub> catalyst, owing to its high OCM performance and thermostability at high temperatures, has become a promising OCM catalyst. The synergy and dispersion of Na<sub>2</sub>WO<sub>4</sub> and Mn<sub>2</sub>O<sub>3</sub> are important factors in improving OCM performance, and the selection of the support has a significant impact on their dispersion and interaction. To enhance the synergistic effect and dispersion of Na<sub>2</sub>WO<sub>4</sub> and Mn<sub>2</sub>O<sub>3</sub>, a TS-1 support doped with varying amounts of Ti was selected for the Mn<sub>2</sub>O<sub>3</sub>–Na<sub>2</sub>WO<sub>4</sub>/<em>x</em>TS-1 (Na–W–Mn/<em>x</em>TS-1) catalyst preparation. The characterization results showed that Ti addition promoted Na<sub>2</sub>WO<sub>4</sub> dispersion and enhanced interactions between Na<sub>2</sub>WO<sub>4</sub> and Mn<sub>2</sub>O<sub>3</sub>. Moreover, Ti doping effectively promoted the generation of active oxygen species and increased the conversion of methane, thereby increasing the C<sub>2</sub> yield. The Na–W–Mn/8%TS-1 catalyst exhibited the highest OCM performance, with a 20.0% C<sub>2</sub> yield and 46.8% CH<sub>4</sub> conversion. The enhanced OCM performance may be caused by the increased dispersion of Na<sub>2</sub>WO<sub>4</sub> and Mn<sub>2</sub>O<sub>3</sub> induced by the atomic-level Ti doping in the TS-1 support, which promoted their interaction and increased the number of lattice oxygen species.</div></div>\",\"PeriodicalId\":66,\"journal\":{\"name\":\"Catalysis Science & Technology\",\"volume\":\"15 8\",\"pages\":\"Pages 2628-2641\"},\"PeriodicalIF\":4.4000,\"publicationDate\":\"2025-02-21\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Catalysis Science & Technology\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/org/science/article/pii/S204447532500111X\",\"RegionNum\":3,\"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":"Catalysis Science & Technology","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/org/science/article/pii/S204447532500111X","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Enhanced oxidative coupling of methane over Mn2O3–Na2WO4/TS-1 catalysts by the Ti induced synergistic effect between Mn2O3 and Na2WO4
Oxidative coupling of methane (OCM) can directly convert natural gas into C2 hydrocarbons (C2H4 and C2H6). The Mn2O3–Na2WO4/SiO2 catalyst, owing to its high OCM performance and thermostability at high temperatures, has become a promising OCM catalyst. The synergy and dispersion of Na2WO4 and Mn2O3 are important factors in improving OCM performance, and the selection of the support has a significant impact on their dispersion and interaction. To enhance the synergistic effect and dispersion of Na2WO4 and Mn2O3, a TS-1 support doped with varying amounts of Ti was selected for the Mn2O3–Na2WO4/xTS-1 (Na–W–Mn/xTS-1) catalyst preparation. The characterization results showed that Ti addition promoted Na2WO4 dispersion and enhanced interactions between Na2WO4 and Mn2O3. Moreover, Ti doping effectively promoted the generation of active oxygen species and increased the conversion of methane, thereby increasing the C2 yield. The Na–W–Mn/8%TS-1 catalyst exhibited the highest OCM performance, with a 20.0% C2 yield and 46.8% CH4 conversion. The enhanced OCM performance may be caused by the increased dispersion of Na2WO4 and Mn2O3 induced by the atomic-level Ti doping in the TS-1 support, which promoted their interaction and increased the number of lattice oxygen species.
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