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新型深共晶溶剂-二氧化硅化学催化剂和新构建的还原酶生物催化剂催化生物质转化为糠醇。

Catalytic valorization of biomass for furfuryl alcohol by novel deep eutectic solvent-silica chemocatalyst and newly constructed reductase biocatalyst.

机构信息

State Key Laboratory of Biocatalysis and Enzyme Engineering, Hubei Collaborative Innovation Center for Green Transformation of Bio-resources, Hubei Key Laboratory of Industrial Biotechnology, School of Life Sciences, Hubei University, Wuhan, Hubei Province, China.

National-Local Joint Engineering Research Center of Biomass Refining and High-Quality Utilization, Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology, Advanced Catalysis and Green Manufacturing Collaborative Innovation Center, School of Pharmacy, Changzhou University, Changzhou, Jiangsu Province, China.

出版信息

Bioresour Technol. 2022 Mar;347:126376. doi: 10.1016/j.biortech.2021.126376. Epub 2021 Nov 18.

Abstract

Chemoenzymatic cascade catalysis using deep eutectic solvent-silica heterogeneous catalyst and reductase biocatalyst was constructed for synthesizing furfuryl alcohol from biomass in one-pot manner. A novel heterogeneous catalyst B:LA-SG(SiO) was firstly prepared by immobilizing deep eutectic solvent Betaine:Lactic acid on silica with sol-gel method using tetraethyl orthosilicate as silicon source. High furfural yield (45.3%) was achieved from corncob with B:LA-SG(SiO) catalyst (2.5 wt%) in water at 170 ˚C for 0.5 h. Possible catalytic mechanism for converting biomass into furfural was proposed. Moreover, one newly constructed recombinant E. coli KF2021 cells containing formate dehydrogenase and reductase was utilized to transform corncob-valorized furfural into furfuralcohol at 97.7% yield at pH 7.5 and 40 ˚C via HCOONa-driven coenzyme regeneration. Such a hybrid process was constructed for tandem chemocatalysis and biocatalysis in a same reactor, potentially reducing the operation cost, which had potential application for valorization of biomass to value-added furans.

摘要

采用深共熔溶剂-硅质非均相催化剂和还原酶生物催化剂的酶化学级联催化,以一锅法从生物质合成糠醇。首次通过溶胶-凝胶法用四乙氧基硅烷作为硅源,将甜菜碱:乳酸深共熔溶剂固定在硅上,制备了新型非均相催化剂 B:LA-SG(SiO)。在水相中,以 B:LA-SG(SiO)催化剂(2.5wt%)在 170℃下反应 0.5h,从玉米芯中获得了 45.3%的高糠醛收率。提出了一种将生物质转化为糠醛的可能催化机制。此外,利用新构建的含有甲酸脱氢酶和还原酶的重组大肠杆菌 KF2021 细胞,在 pH 7.5 和 40℃下,通过 HCOONa 驱动辅酶再生,以 97.7%的收率将玉米芯增值的糠醛转化为糠醇。在同一个反应器中构建了这种串联的化学催化和生物催化的杂化工艺,有望降低操作成本,为生物质增值为有价值的呋喃提供了潜在的应用。

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