Benzene, toluene, and p-xylene (BTpX) are among the most important commodity chemicals, but their productions still heavily rely on fossil resources and thus pose serious environmental burdens and energy crisis. Herein, the tandem upgrading of bio-furans is reported to high-yield BTpX by rationally constructing a versatile Pt₁Sn₁ intermetallic coupling ordered-mesoporous SnO₂ (OM-SnO₂) catalyst. It is shown that with increasing reduction temperature from 200 to 350 °C, Pt nanoparticles (NPs) are first formed on OM-SnO₂, then converted to Pt₃Sn₁ intermetallic nanoparticles (iNPs), and finally to Pt₁Sn₁ iNPs with a gradually-thickened SnO₂ overlayer. Impressively, the Pt₁Sn₁ iNPs and defect-rich OM-SnO₂ in the optimized Pt@OM-SnO₂ can serve as the highly-active species for the hydrogenolysis of 5-hydroxymethylfuran to 2,5-dimethylfuran and the aromatization of 2,5-dimethylfuran with acrylic acid to p-xylene, affording the highest yields of 99.1% and 96.1%, respectively. More importantly, it can perfectly realize the tandem upgrading of furan, furfural and 5-hydroxymethylfuran to benzene, toluene and p-xylene with high yields of 94.6%, 94.2% and 95.2%, respectively, representing a new tandem catalytic system to realize the high-yield BTpX productions from their corresponding bio-furans. This catalyst also shows good recyclability and excellent scalability, which together with its superior activity/selectivity suggest a high potential for sustainable BTpX productions.

中文翻译：

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通过 Pt1Sn1 金属间化合物偶联有序介孔 SnO2 催化剂将生物呋喃串联升级为苯、甲苯和对二甲苯


苯、甲苯和对二甲苯 （BTpX） 是最重要的商品化学品之一，但它们的生产仍然严重依赖化石资源，因此造成严重的环境负担和能源危机。在此，通过合理构建多功能的 Pt₁Sn₁ 金属间化合物耦合有序介孔 SnO₂ （OM-SnO₂） 催化剂，报道了生物呋喃的串联升级为高产率 BTpX。结果表明，随着还原温度从 200°C 增加到 350°C，Pt 纳米颗粒 （NPs） 首先在 OM-SnO₂ 上形成，然后转化为 Pt₃Sn₁ 金属间化合物纳米颗粒 （iNPs），最后转化为 Pt₁Sn₁ iNPs，具有逐渐增厚的 SnO₂ 外层。令人印象深刻的是，优化的 Pt@OM-SnO₂ 中的 Pt₁Sn₁ iNPs 和富含缺陷的 OM-SnO₂ 可以作为 5-羟甲基呋喃氢解为 2,5-二甲基呋喃和 2,5-二甲基呋喃与丙烯酸的芳构化反应为对二甲苯的高活性物质，分别获得 99.1% 和 96.1% 的最高产率。更重要的是，它可以完美地实现呋喃、糠醛和 5-羟甲基呋喃向苯、甲苯和对二甲苯的串联升级，分别高产率为 94.6%、94.2% 和 95.2%，代表了一种新的串联催化体系，可以从相应的生物呋喃中实现高产率 BTpX。该催化剂还表现出良好的可回收性和出色的可扩展性，再加上其卓越的活性/选择性，表明 BTpX 可持续生产具有很大的潜力。