Experimental and Kinetic Study on Lignin Depolymerization in Water/Formic Acid System.
Experimental and Kinetic Study on Lignin Depolymerization in Water/Formic Acid System.
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水/甲酸体系中木质素解聚的实验及动力学研究
DOI：
10.3390/ijms18102082
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发表时间：
2017-10-01
影响因子：
5.6
通讯作者：
Shen D
中科院分区：
文献类型：
--
作者：
Wang Q;Guan S;Shen D
研究了微波辅助下黑液木质素在甲酸中的解聚反应，重点研究了生物油1（主要为芳香族单体）和生物油2（主要为芳香族低聚物）液相组分的产率及其具体组分的分布。生物油1（9.69%）和生物油2（54.39%）在160℃条件下反应30 min，收率最高。采用气相色谱-质谱联用仪（GC-MS）和基质辅助激光解吸/电离飞行时间质谱联用仪（MALDI-TOF MS）分别鉴定了生物油1和生物油2的化学成分。结果表明，1-（4-羟基-3-甲氧基苯基）和1-（4-羟基-3,5-二甲氧基苯基）是生物油中最主要的两种化合物。MALDI-TOF质谱鉴定的分子量为328、342、358、378、394、424和454的芳香低聚物的产量与反应温度有很大的关系。提出了微波辅助下木质素酸性溶剂分解的两阶段动力学模型，其中第一阶段主要是木质素解聚成单体和低聚物，活化能为40.27 kJ·mol−1；第二阶段主要是第一阶段产物的再聚合，活化能为49.18 kJ·mol−1。
Microwave-assisted depolymerization of black-liquor lignin in formic acid was studied, concentrating on the yield of liquid fractions as bio-oil 1 (mainly aromatic monomers) and bio-oil 2 (mainly aromatic oligomers) and the distribution of the specific compositions. Bio-oil 1 (9.69%) and bio-oil 2 (54.39%) achieved their maximum yields under 160 °C with the reaction time of 30 min. The chemical compositions of bio-oil 1 and bio-oil 2 were respectively identified by means of Gas Chromatography-Mass Spectrometer (GC-MS) and Matrix-assisted laser desorption/ionization time-of-flight mass spectrometry (MALDI-TOF MS). Ethanone, 1-(4-hydroxy-3-methoxyphenyl) and Ethanone, 1-(4-hydrox-3,5-dimethoxyphenyl) were evidenced to be the two prominent compounds in bio-oil 1. Production of aromatic oligomers with the molecular weight of 328, 342, 358, 378, 394, 424 and 454 identified by MALDI-TOF MS was substantially tuned with the reaction temperature. A two-separate-stage kinetic model was proposed to describe the acidic solvolysis of lignin assisted by microwave heating, where the first stage is dominated by the depolyerization of lignin to monomers and oligomers with the activation energy of 40.27 kJ·mol−1, and the second stage with the activation energy of 49.18 kJ·mol−1 is mainly ascribed to the repolymerization of first-stage produced compounds.
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