Zhai Qiaolong, Li Jie, Miao Kangze, Song Yunhao, Yang Shaoqi, Zhao Shuheng, Lu Yanju, Hu Jianjun
Key Laboratory of New Materials and Facilities for Rural Renewable Energy of Ministry of Agriculture and Rural Affairs, College of Mechanical & Electrical Engineering, Henan International Joint Laboratory of Biomass Energy and Nanomaterials, Henan Agricultural University, Zhengzhou 450002, China.
Key Laboratory of New Materials and Facilities for Rural Renewable Energy of Ministry of Agriculture and Rural Affairs, College of Mechanical & Electrical Engineering, Henan International Joint Laboratory of Biomass Energy and Nanomaterials, Henan Agricultural University, Zhengzhou 450002, China.
Int J Biol Macromol. 2025 Feb;290:138736. doi: 10.1016/j.ijbiomac.2024.138736. Epub 2024 Dec 14.
This study developed a "one-pot" three-stage process using a "multifunctional" deep eutectic solvent (DES) containing choline chloride (ChCl), ethylene glycol (EG), and protonic acids for the production of phenolic monomers, furfural, and glucose. In the first stage, the DES effectively dissolved over 70 % of lignin and 78 % of hemicellulose while preserving aryl ether bonds in lignin due to the grafting of EG onto the aryl ether bonds. Concurrently, the retention of a near-quantitative amount of cellulose led to a glucose yield of >80 % after enzymatic saccharification. In the next stage, the DES enabled the catalytic depolymerization of lignin using a Ru/C catalyst at mild temperatures and atmospheric pressure, eliminating the need for an external hydrogen source and yielding G/S-propyl and G/S-propenyl monomers at 13.8 %. Additionally, the ratio of ChCl to EG in the DES could regulate the composition and selectivity of the phenolic monomers. Following this, the hemicellulose sugars dissolved in the DES underwent catalytic hydrolysis in a DES/water system, achieving a furfural yield of 36.4 % under optimized conditions. The results of this study offer important insights into the valorization of lignocellulose in "one-pot" under mild conditions, thereby advancing the field of biorefining.
本研究开发了一种“一锅法”三阶段工艺,使用含有氯化胆碱(ChCl)、乙二醇(EG)和质子酸的“多功能”低共熔溶剂(DES)来生产酚类单体、糠醛和葡萄糖。在第一阶段,DES有效地溶解了70%以上的木质素和78%的半纤维素,同时由于EG接枝到芳基醚键上,保留了木质素中的芳基醚键。同时,近乎定量的纤维素得以保留,酶解糖化后葡萄糖产率>80%。在下一阶段,DES能够在温和温度和常压下使用Ru/C催化剂对木质素进行催化解聚,无需外部氢源,G/S-丙基和G/S-丙烯基单体产率为13.8%。此外,DES中ChCl与EG的比例可调节酚类单体的组成和选择性。在此之后,溶解在DES中的半纤维素糖在DES/水体系中进行催化水解,在优化条件下糠醛产率达到36.4%。本研究结果为温和条件下“一锅法”木质纤维素的增值利用提供了重要见解,从而推动了生物精炼领域的发展。