Cu-xMo /SiO2催化剂上马来酸酐深度加氢一锅法合成1,4-丁二醇

IF 4.4 3区 化学 Q2 CHEMISTRY, PHYSICAL Catalysis Science & Technology Pub Date : 2024-11-05 DOI:10.1039/d4cy01006j
Kai Cui , Jiaming Yang , Yuli Jing , Junwen Chen , Chen Zhao , Peng Wu , Xiaohong Li
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引用次数: 0

摘要

可持续性问题导致生物降解塑料的1,4-丁二醇(BDO)单体逐渐扩大市场,以取代传统塑料。马来酸酐(MA)可以由生物基糠醛或果糖氧化得到。虽然MA加氢可以产生琥珀酸酐(SA)、γ-丁内酯(GBL)、BDO和四氢呋喃(THF)等一系列产物,但迄今为止文献中很少报道MA在温和条件下一锅深度加氢制BDO或THF。本文报道了在Cu-0.03Mo /SiO2催化剂上,MA一锅深度加氢制备BDO, MA转化率达到100%,BDO产率达到88.3%。Cu-0.03Mo /SiO2催化剂也表现出良好的长期稳定性,在160 h的流动时间测试中,活性和BDO选择性没有明显下降。在Cu/SiO2催化剂中掺杂适量的Mo,可以调节Cu0/Cu+的分布,调节Cu - SiO2与表面酸度的相互作用,使氢、MA及相关中间体的活化趋于平衡,并限制副反应的发生。该研究为非贵金属铜基催化剂绿色合成BDO提供了潜力。
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One-pot synthesis of 1,4-butanediol via the deep hydrogenation of maleic anhydride over Cu–xMo/SiO2 catalysts†
Sustainability issues have led to a gradual market expansion for the 1,4-butanediol (BDO) monomer of the biodegradable plastics to replace conventional plastics. Maleic anhydride (MA) can be derived from the oxidation of bio-based furfural or fructose. Although the hydrogenation of MA can produce a series of products, including succinic anhydride (SA), γ-butyrolactone (GBL), BDO and tetrahydrofuran (THF), the one-pot deep hydrogenation of MA to BDO or THF under mild conditions has been rarely reported in the literature until now. Herein, we report the production of BDO from the one-pot deep hydrogenation of MA over a Cu–0.03Mo/SiO2 catalyst, achieving 100% MA conversion and 88.3% BDO yield. The Cu–0.03Mo/SiO2 catalyst also showed good long-term stability without obvious loss in activity or BDO selectivity during a 160 h time-on-stream test. Doping Mo to Cu/SiO2 catalysts in an optimal amount adjusted the distribution of Cu0/Cu+ species and modulated the interaction of Cu–SiO2 and surface acidity, so that the activation of hydrogen, MA and relevant intermediates can become balanced, in addition to the restriction of side-reactions. This study provides potential for the green synthesis of BDO with non-precious Cu-based catalysts.
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来源期刊
Catalysis Science & Technology
Catalysis Science & Technology CHEMISTRY, PHYSICAL-
CiteScore
8.70
自引率
6.00%
发文量
587
审稿时长
1.5 months
期刊介绍: A multidisciplinary journal focusing on cutting edge research across all fundamental science and technological aspects of catalysis. Editor-in-chief: Bert Weckhuysen Impact factor: 5.0 Time to first decision (peer reviewed only): 31 days
期刊最新文献
Back cover Polystyrene-bound AlCl3 - a catalyst for the solvent-free synthesis of aryl-substituted tetrazoles. Back cover Inside back cover Back cover
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