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Catalytic conversion of glucose to 5-hydroxymethyfural over Fe/β zeolites with extra-framework isolated Fe species in a biphasic reaction system
Biomass & Bioenergy ( IF 5.8 ) Pub Date : 2017-12-18 , DOI: 10.1016/j.biombioe.2017.12.007
Haian Xia , Hong Hu , Siquan Xu , Kehao Xiao , Songlin Zuo

A series of Fe/β zeolite catalysts with various Fe/Al ratios were prepared by liquid ion-exchanged method and were characterized by N2 adsorption, XRD, UV–Vis DRS, EPR, NH3-TPD, and FTIR of pyridine adsorption techniques. The catalysts were used to catalyze the transformation of glucose into 5-hydorxymethyfural (HMF) in a biphasic reaction system under mild reaction conditions. The Fe/β catalysts with Lewis acidic Fe sites is able to effectively improve the HMF yield compared to H-β zeolite under identical reaction conditions, which is ascribed to the enhanced isomerization activity of glucose-to-fructose by Lewis acidic Fe species. Moreover, the Fe/Al ratio had a remarkable impact on the conversion of glucose and the yield of HMF, indicating that the synergetic effect of Lewis and Brønsted acid sites is critical to achieving high HMF yield. Under optimal reaction conditions, Fe/β-0.06 catalyst afforded 61% HMF yield at glucose conversion of 95% after the reaction of 90 min at 120 °C, which is one of the most effective catalysts for the conversion of glucose into HMF in a biphasic medium up to now. Furthermore, extra-framework isolated Fe species bound to the framework Al sites, are most likely the active sites for the isomerization of glucose-to-fructose in the conversion of glucose. The catalysts were very stable and could be reused at least five runs without significant loss in the catalytic activity.



中文翻译:

Fe /β分子筛在双相反应体系中将葡萄糖催化转化为Fe /β沸石上的5-羟基甲基糠醛

通过液离子交换法制备了一系列具有不同Fe / Al比的Fe /β沸石催化剂,并以N 2吸附,XRD,UV-Vis DRS,EPR,NH 3为特征进行了表征。-TPD和吡啶的FTIR吸附技术。在温和的反应条件下,该催化剂用于在双相反应系统中催化葡萄糖转化为5-羟甲基糠醛(HMF)。在相同的反应条件下,具有路易斯酸性Fe位点的Fe /β催化剂与H-β沸石相比能够有效提高HMF产率,这归因于路易斯酸性Fe物种增强了葡萄糖到果糖的异构化活性。此外,Fe / Al比对葡萄糖的转化率和HMF的收率有显着影响,表明路易斯酸和布朗斯台德酸位点的协同作用对于实现高HMF收率至关重要。在最佳反应条件下,Fe /β-0.06催化剂在120°C下反应90分钟后,在葡萄糖转化率为95%时,HMF收率为61%,迄今为止,它是在双相介质中将葡萄糖转化为HMF的最有效催化剂之一。此外,与框架A1位点结合的框架外分离的Fe物种最有可能是葡萄糖转化中葡萄糖到果糖的异构化的活性位点。催化剂非常稳定,可以重复使用至少五次,而催化活性没有明显损失。

更新日期:2017-12-19
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