Jiaqi Yan, Weiwen Fu, Kuiyi You, Fangfang Zhao, He’an Luo
{"title":"介孔固定化 BiCl3 硅酸作为稳定的路易斯酸催化剂，用于在温和条件下从邻二甲苯与二氧化氮的硝化反应中选择性合成 4-硝基邻二甲苯","authors":"Jiaqi Yan, Weiwen Fu, Kuiyi You, Fangfang Zhao, He’an Luo","doi":"10.1007/s11144-024-02698-8","DOIUrl":null,"url":null,"abstract":"<p>A solvent-free, acid-free, and efficient strategy was developed for the selective preparation of 4-nitro-o-xylene (4-NOX) from the catalytic nitration of o-xylene with NO<sub>2</sub> mediated O<sub>2</sub> over BiCl<sub>3</sub> immobilized silicic acid catalyst (BiCl<sub>3</sub>-SA). The results indicated that the Lewis acid BiCl<sub>3</sub>-SA conjoined NO<sub>2</sub>–O<sub>2</sub> as a composite system synergistically promotes o-xylene conversion and 4-NOX selectivity. Under optimal conditions, 52.4% of o-xylene conversion with 68.4% 4-NOX selectivity was obtained at 35 °C. The characterization demonstrated that the highly dispersed metal Bi species form stable chemical bonds with the SA surface, which can effectively inhibit the loss of metal species and generate abundant acid sites. The developed catalyst is not only inexpensive but also has excellent stability and catalytic performance. Furthermore, a plausible mechanism for the catalytic nitration of o-xylene using NO<sub>2</sub> as a nitration agent over BiCl<sub>3</sub>-SA was proposed. This work provides an eco-friendly and practical protocol for improving desirable 4-NOX selectivity and reducing the discharge of acidic wastewater, with potential application prospects.</p><h3 data-test=\"abstract-sub-heading\">Graphical abstract</h3>","PeriodicalId":1,"journal":{"name":"Accounts of Chemical Research","volume":null,"pages":null},"PeriodicalIF":16.4000,"publicationDate":"2024-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Mesoporous BiCl3 immobilized silicic acid as a stabilized Lewis acid catalyst for the selective synthesis of 4-nitro-o-xylene from the nitration of o-xylene with NO2 under mild conditions\",\"authors\":\"Jiaqi Yan, Weiwen Fu, Kuiyi You, Fangfang Zhao, He’an Luo\",\"doi\":\"10.1007/s11144-024-02698-8\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>A solvent-free, acid-free, and efficient strategy was developed for the selective preparation of 4-nitro-o-xylene (4-NOX) from the catalytic nitration of o-xylene with NO<sub>2</sub> mediated O<sub>2</sub> over BiCl<sub>3</sub> immobilized silicic acid catalyst (BiCl<sub>3</sub>-SA). The results indicated that the Lewis acid BiCl<sub>3</sub>-SA conjoined NO<sub>2</sub>–O<sub>2</sub> as a composite system synergistically promotes o-xylene conversion and 4-NOX selectivity. Under optimal conditions, 52.4% of o-xylene conversion with 68.4% 4-NOX selectivity was obtained at 35 °C. The characterization demonstrated that the highly dispersed metal Bi species form stable chemical bonds with the SA surface, which can effectively inhibit the loss of metal species and generate abundant acid sites. The developed catalyst is not only inexpensive but also has excellent stability and catalytic performance. Furthermore, a plausible mechanism for the catalytic nitration of o-xylene using NO<sub>2</sub> as a nitration agent over BiCl<sub>3</sub>-SA was proposed. This work provides an eco-friendly and practical protocol for improving desirable 4-NOX selectivity and reducing the discharge of acidic wastewater, with potential application prospects.</p><h3 data-test=\\\"abstract-sub-heading\\\">Graphical abstract</h3>\",\"PeriodicalId\":1,\"journal\":{\"name\":\"Accounts of Chemical Research\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":16.4000,\"publicationDate\":\"2024-07-30\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Accounts of Chemical Research\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1007/s11144-024-02698-8\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Accounts of Chemical Research","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1007/s11144-024-02698-8","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Mesoporous BiCl3 immobilized silicic acid as a stabilized Lewis acid catalyst for the selective synthesis of 4-nitro-o-xylene from the nitration of o-xylene with NO2 under mild conditions
A solvent-free, acid-free, and efficient strategy was developed for the selective preparation of 4-nitro-o-xylene (4-NOX) from the catalytic nitration of o-xylene with NO2 mediated O2 over BiCl3 immobilized silicic acid catalyst (BiCl3-SA). The results indicated that the Lewis acid BiCl3-SA conjoined NO2–O2 as a composite system synergistically promotes o-xylene conversion and 4-NOX selectivity. Under optimal conditions, 52.4% of o-xylene conversion with 68.4% 4-NOX selectivity was obtained at 35 °C. The characterization demonstrated that the highly dispersed metal Bi species form stable chemical bonds with the SA surface, which can effectively inhibit the loss of metal species and generate abundant acid sites. The developed catalyst is not only inexpensive but also has excellent stability and catalytic performance. Furthermore, a plausible mechanism for the catalytic nitration of o-xylene using NO2 as a nitration agent over BiCl3-SA was proposed. This work provides an eco-friendly and practical protocol for improving desirable 4-NOX selectivity and reducing the discharge of acidic wastewater, with potential application prospects.
期刊介绍：
Accounts of Chemical Research presents short, concise and critical articles offering easy-to-read overviews of basic research and applications in all areas of chemistry and biochemistry. These short reviews focus on research from the author’s own laboratory and are designed to teach the reader about a research project. In addition, Accounts of Chemical Research publishes commentaries that give an informed opinion on a current research problem. Special Issues online are devoted to a single topic of unusual activity and significance.
Accounts of Chemical Research replaces the traditional article abstract with an article "Conspectus." These entries synopsize the research affording the reader a closer look at the content and significance of an article. Through this provision of a more detailed description of the article contents, the Conspectus enhances the article's discoverability by search engines and the exposure for the research.
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