Catalytic production of 1,4-pentanediol from furfural in a fixed-bed system under mild conditions

Catalytic production of 1,4-pentanediol from furfural in a fixed-bed system under mild conditions
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温和条件下固定床系统催化糠醛生产1,4-戊二醇

DOI:
10.1039/d0gc00233j
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发表时间:
2020-06-07
期刊:
影响因子:
9.8
通讯作者:
Zhang, Tao
Zhang, Tao
中科院分区:
化学1区
文献类型:
--
作者:
Liu, Qiaoyun;Qiao, Botao;Zhang, Tao

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糠醛是最重要的生物质衍生化学品之一。它的大规模可用性要求探索新的转换方法,以进一步稳定价格。在这里,我们报告了使用Amberlyst-15和Ru-FeOx/AC催化剂的组合将糠醛直接一步转化为1,4-戊二醇(1,4-Peds)。研究发现,适量的FeOx的引入,大大改善了Ru的分散性,降低了刘易斯酸性。XPS和H-2-TPR均表明Ru与Fe之间存在电子转移,电子间的相互作用促进了Ru和Fe物种的还原。当与Amberlyst-15组合使用时,Ru-6.3FeO(x)/AC催化剂提供最佳性能,1,4-PeD产率为86%;相比之下,不含FeOx的Ru/AC仅产生乙酰丙酸作为主要产物,证明了酸/金属平衡在糠醛一锅转化为1,4-PeD中的关键作用。此外,这种双功能催化剂在175小时的运转时间内表现出优异的耐久性。
Furfural is one of the most important biomass-derived chemicals. Its large-scale availability calls for the exploration of new transformation methods for further valorization. Here we report on the direct, one-step conversion of furfural into 1,4-pentanediols (1,4-PeDs) using a combination of Amberlyst-15 and Ru-FeOx/AC catalysts. It is interesting to find that the introduction of a suitable amount of FeOx results in a great improvement in the dispersion of Ru and a decrease in the Lewis acidity. Both XPS and H-2-TPR show that there is electron transfer from Ru to Fe, and the electronic interaction facilitates the reduction of both Ru and Fe species. When used in combination with Amberlyst-15, the Ru-6.3FeO(x)/AC catalyst afforded the best performance with a 1,4-PeD yield of 86%; by contrast, Ru/AC free of FeOx only gave levulinic acid as the major product, demonstrating the key role of the acid/metal balance in the one-pot conversion of furfural to 1,4-PeD. Moreover, such a dual catalyst exhibited excellent durability within 175 h time-on-stream.