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

IF 16.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Accounts of Chemical Research Pub Date : 2024-07-30 DOI:10.1007/s11144-024-02698-8

Jiaqi Yan, Weiwen Fu, Kuiyi You, Fangfang Zhao, He’an Luo

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Abstract

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.

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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

研究人员开发了一种无溶剂、无酸和高效的策略，用于在固定化硅酸催化剂 BiCl3（BiCl3-SA）上以 NO2 为介质的 O2 催化硝化邻二甲苯，从而选择性地制备 4-硝基邻二甲苯（4-NOX）。结果表明，路易斯酸 BiCl3-SA 与 NO2-O2 组成的复合体系能协同促进邻二甲苯的转化和 4-NOX 的选择性。在最佳条件下，35 ℃ 时邻二甲苯转化率为 52.4%，4-NOX 选择性为 68.4%。表征结果表明，高度分散的金属 Bi 物种与 SA 表面形成稳定的化学键，可有效抑制金属物种的流失，并产生丰富的酸性位点。所开发的催化剂不仅价格低廉，而且具有优异的稳定性和催化性能。此外，还提出了以 NO2 为硝化剂在 BiCl3-SA 上催化硝化邻二甲苯的合理机理。这项工作为提高理想的 4-NOX 选择性和减少酸性废水排放提供了一种环保实用的方案，具有潜在的应用前景。

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来源期刊

Accounts of Chemical Research 化学-化学综合

CiteScore

31.40

自引率

1.10%

发文量

312

审稿时长

2 months

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.