通过 Pt1Sn1 金属间偶联有序介孔 SnO2 催化剂串联提纯生物呋喃至苯、甲苯和对二甲苯

IF 27.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Advanced Materials Pub Date : 2024-11-20 DOI:10.1002/adma.202415295
Shoukang Xiao, Li Wang, Liyu Chen, Yingwei Li, Kui Shen
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引用次数: 0

摘要

苯、甲苯和对二甲苯(BTpX)是最重要的商品化学品之一,但其生产仍然严重依赖化石资源,因此带来了严重的环境负担和能源危机。本文报道了通过合理构建多功能 Pt1Sn1 金属间偶联有序多孔 SnO2(OM-SnO2)催化剂,串联提纯生物呋喃,从而高产 BTpX。研究表明,随着还原温度从 200 ℃ 升至 350 ℃,铂纳米颗粒(NPs)首先在 OM-SnO2 上形成,然后转化为 Pt3Sn1 金属间纳米颗粒(iNPs),最后转化为 Pt1Sn1 iNPs,其上的 SnO2 覆盖层逐渐增厚。令人印象深刻的是,优化后的 Pt@OM-SnO2 中的 Pt1Sn1 iNPs 和富含缺陷的 OM-SnO2 可作为高活性物种,用于将 5-羟甲基呋喃氢解为 2,5-二甲基呋喃,以及将 2,5-二甲基呋喃与丙烯酸芳构化为对二甲苯,最高产率分别为 99.1%和 96.1%。更重要的是,它能完美地实现呋喃、糠醛和 5-羟甲基呋喃向苯、甲苯和对二甲苯的串联升级,收率分别高达 94.6%、94.2% 和 95.2%,是一种新型串联催化体系,可实现从相应的生物呋喃高产 BTpX。这种催化剂还具有良好的可回收性和出色的可扩展性,加上其卓越的活性/选择性,表明它在可持续生产 BTpX 方面具有很大的潜力。
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Tandem Upgrading of Bio-Furans to Benzene, Toluene, and p-xylene by Pt1Sn1 Intermetallic Coupling Ordered Mesoporous SnO2 Catalyst
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.
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来源期刊
Advanced Materials
Advanced Materials 工程技术-材料科学:综合
CiteScore
43.00
自引率
4.10%
发文量
2182
审稿时长
2 months
期刊介绍: Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.
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