One-pot production of oxygenated monomers and selectively oxidized lignin from biomass based on plasma electrolysis
One-pot production of oxygenated monomers and selectively oxidized lignin from biomass based on plasma electrolysis
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基于等离子体电解的生物质一锅法生产含氧单体和选择性氧化木质素
DOI：
10.1039/d1gc03315h
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发表时间：
2021
期刊：
影响因子：
9.8
通讯作者：
Bai, Xianglan
中科院分区：
文献类型：
--
作者：
A, Lusi;Radhakrishnan, Harish;Hu, Hui;Bai, Xianglan
在此，我们报告了一种新的方法，以获得含氧化合物和高品质的木质素从生物质在一锅使用一个单一的步骤过程。以硫酸为电解液，采用高压交流电对红橡进行等离子体电解，得到γ-戊内酯。红橡木被完全溶解，产生左旋葡萄糖酮和糠醛作为两个主要单体，分别高达44.9摩尔%和98.0摩尔%的产率。在转化过程中，还同时产生高纯度的氧化木质素。使用热解方法评估的等离子体电解衍生的木质素的增值潜力表明，这种木质素的解聚可以产生比天然木质素或在常规溶剂分解过程中分离的木质素显著更高的酚类单体产率。我们的研究表明，在等离子体电解过程中，天然木质素的苄基碳被选择性地修饰，以限制单元间C-C键的形成，显着改善随后的木质素对芳香族单体的稳定化。总的来说，这项研究证明了一种简单的绿色方法，可以在不使用昂贵的催化剂或繁琐的生物质分馏的情况下改善化学品生产。本研究为木质素的改性提供了一种新的高效途径。
Herein, we report a novel method to obtain oxygenated chemicals and high-quality lignin from biomass in one-pot using a single step process. Plasma electrolysis of red oak was conducted by applying high-voltage alternating current electricity in γ-valerolactone using sulfuric acid as the electrolyte. Red oak was completely solubilized to produce levoglucosenone and furfural as the two major monomers with the respective yields of up to 44.9 mol% and 98.0 mol%. During the conversion, an oxidized lignin was also simultaneously produced in high purity. The valorization potential of the plasma electrolysis-derived lignin evaluated using the pyrolysis method showed that depolymerization of this lignin could produce significantly higher yields of phenolic monomers than the natural lignin or the lignin isolated during conventional solvolysis. Our investigation showed that benzylic carbon of the natural lignin was selectively modified during plasma electrolysis to limit the formation of interunit C–C bonds, significantly improving the subsequent lignin valorization to aromatic monomers. Overall, this study demonstrated a simple green approach to improve chemical production without using costly catalysts or tedious biomass fractionation. This study also presented a novel and highly efficient way to modify lignin for enhanced valorization.