Elucidation of the interaction effects of cellulose, hemicellulose and lignin during degradative solvent extraction of lignocellulosic biomass
Elucidation of the interaction effects of cellulose, hemicellulose and lignin during degradative solvent extraction of lignocellulosic biomass
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木质纤维素生物质降解溶剂提取过程中纤维素、半纤维素和木质素相互作用的阐明
DOI：
10.1016/j.fuel.2022.125141
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发表时间：
2022
期刊：
影响因子：
7.4
通讯作者：
Qiang Liao
中科院分区：
文献类型：
--
作者：
Xianqing Zhu;Man Liu;Qintao Sun;Jingjing Ma;Ao Xia;Yun Huang;Xun Zhu;Qiang Liao
降解溶剂萃取（DSE）方法是近年来发展起来的一种将木质纤维素生物质废弃物脱木素和提质为具有多种附加值应用的高质量提取物的方法。木质纤维素生物质主要由纤维素、半纤维素和木质素组成，这三种组分在DSE过程中的相互作用尚不清楚，需要阐明。因此，在本研究中，合成组分混合物首先用模型化合物制备了纤维素/半纤维素（CH）、纤维素/木质素（CL）和半纤维素/木质素（HL（纤维素、半纤维素和木质素），在相同的操作条件下，比较了DSE过程中各组分混合物的转化特性和各组分的叠加特性，揭示了DSE过程中各组分之间的相互作用。三个组成部分。纤维素、半纤维素和木质素的提取率分别为44.16%、27.4%和18.25%，表明纤维素对提取物（目标产物）的形成贡献最大，而半纤维素和木质素的贡献较小。纤维素/木质素和半纤维素/木质素混合物中观察到显著的相互作用，而纤维素和半纤维素之间的相互作用效应相对较小。纤维素、半纤维素和木质素之间的相互作用强度为HL > CL > CH。纤维素/木质素和半纤维素/木质素之间的相互作用促进了木质素的热降解。具体地，半纤维素和木质素混合物之间的相互作用使残余物的产率降低了9.26%。通过对DSE产物的详细表征，探讨并揭示了三组分间的相互作用机理。三种组分之间的相互作用可以促进气体产物（主要是CO2）的产生，表明三种组分之间的相互作用显著促进了脱羧反应。三种组分中有两种组分之间的相互作用均抑制了芳构化反应，降低了萃取物的芳香度。在纤维素/木质素或半纤维素/木质素混合物的DSE过程中，纤维素或半纤维素分解产生的小分子自由基可以占据木质素碎片上的活性位点，从而显著抑制不同木质素碎片之间的缩合反应。这些相互作用导致纤维素/木质素或半纤维素/木质素混合物在DSE过程中的提取物产率和残渣产率降低。
The degradative solvent extraction (DSE) method has been recently developed to deoxygenate and upgrade lignocellulosic biomass wastes into high-quality extracts with a variety of value-added applications. Lignocellulosic biomass is mainly composed of cellulose, hemicellulose and lignin, and the interaction of the three components during the DSE process still remains unclear and needs to be elucidated. Therefore, in this study, the synthetic component mixtures (cellulose/hemicellulose (CH), cellulose/lignin (CL) and hemicellulose/lignin (HL)) were firstly prepared with the model compounds (cellulose, hemicellulose and lignin), and the conversion characteristics of the component mixtures and the superposition of individual component during the DSE process under the same operating conditions were compared to reveal the interaction effect between the three components. The extract yields of cellulose, hemicellulose and lignin were 44.16%, 27.4% and 18.25% respectively, indicating that cellulose contributed mostly to the formation of the extract (the target product) compared with hemicellulose and lignin. Significant interactions were observed for cellulose/lignin and hemicellulose/lignin mixtures, while the interaction effect between cellulose and hemicellulose was relatively small. The interaction intensity between cellulose, hemicellulose and lignin was in the order of HL > CL > CH. The interaction between cellulose/lignin and hemicellulose/lignin promoted the thermal degradation of lignin. Specifically, the interaction between the hemicellulose and lignin mixture reduced the yield of residue by 9.26%. The interaction mechanism between the three components was discussed and revealed based on the detailed characterization of the DSE products. The interaction between the three components could facilitate the production of gaseous products (mainly CO2), indicating that the interaction between the three components significantly promoted the decarboxylation reaction. The interaction between two of the three components all inhibited the aromatization reaction and reduced the aromaticity of the extracts. During the DSE process of cellulose/lignin or hemicellulose/lignin mixtures, the small-molecular free radicals generated by the decomposition of cellulose or hemicellulose could occupy the active sites on lignin fragments, leading to the significant inhibition of the condensation reactions between different lignin fragments. These interactions leaded to the decrease of the extract yields and residue yields during the DSE process of cellulose/lignin or hemicellulose/lignin mixtures.
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