Predicting lignin depolymerization yields from quantifiable properties using fractionated biorefinery lignins
Predicting lignin depolymerization yields from quantifiable properties using fractionated biorefinery lignins
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使用分馏生物精炼木质素根据可量化特性预测木质素解聚产量
DOI：
10.1039/c7gc02023f
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发表时间：
2017
期刊：
影响因子：
--
通讯作者：
Hodge, David B.
中科院分区：
文献类型：
--
作者：
Phongpreecha, Thanaphong;Hool, Nicholas C.;Stoklosa, Ryan J.;Klett, Adam S.;Foster, Cliff E.;Bhalla, Aditya;Holmes, Daniel;Thies, Mark C.;Hodge, David B.
木质素解聚成高收率和高选择性的芳香族单体对于整合生物精炼过程中的许多木质素增值策略的经济可行性是必不可少的。重要的是，木质素源的质量和性质在影响转化化学中起着至关重要的作用，但木质素性质和木质素对解聚的敏感性之间的这种关系尚未完全建立。在这项研究中，我们定量地证明了预处理过程对木质素性质的不利影响，特别是β-O-4含量，限制了芳香族单体的高产率，使用三种木质素解聚方法：硫代酸解，氢解和氧化。通过对碱溶木质白杨的pH分级，研究表明，即使在预处理后，木质素的性质，即β-O-4键、酚羟基、分子量和S/G比之间也表现出很强的相关性。此外，这些性质的差异导致使用三种解聚技术的芳族单体产率的明显趋势。基于碱木质素性质的相互依赖性及其对解聚的敏感性，开发了用于预测单体产率的模型，并通过定量硫代酸解验证了解聚。这些结果突出了木质素性质对于它们对于醚裂解解聚过程的适用性的重要性，因为理论单体产率作为β-O-4含量的二阶函数而增长。因此，本研究鼓励并为未来的研究提供了参考工具，以确定木质素优先生物质预处理和木质素增值的新方法，强调保持木质素的质量，除了专注于优化反应条件和催化剂的选择。
Lignin depolymerization to aromatic monomers with high yields and selectivity is essential for the economic feasibility of many lignin-valorization strategies within integrated biorefining processes. Importantly, the quality and properties of the lignin source play an essential role in impacting the conversion chemistry, yet this relationship between lignin properties and lignin susceptibility to depolymerization is not well established. In this study, we quantitatively demonstrate how the detrimental effect of a pretreatment process on the properties of lignins, particularly β-O-4 content, limit high yields of aromatic monomers using three lignin depolymerization approaches: thioacidolysis, hydrogenolysis, and oxidation. Through pH-based fractionation of alkali-solubilized lignin from hybrid poplar, this study demonstrates that the properties of lignin, namely β-O-4 linkages, phenolic hydroxyl groups, molecular weight, and S/G ratios exhibit strong correlations with each other even after pretreatment. Furthermore, the differences in these properties lead to discernible trends in aromatic monomer yields using the three depolymerization techniques. Based on the interdependency of alkali lignin properties and its susceptibility to depolymerization, a model for the prediction of monomer yields was developed and validated for depolymerization by quantitative thioacidolysis. These results highlight the importance of the lignin properties for their suitability for an ether-cleaving depolymerization process, since the theoretical monomer yields grows as a second order function of the β-O-4 content. Therefore, this research encourages and provides a reference tool for future studies to identify new methods for lignin-first biomass pretreatment and lignin valorization that emphasize preservation of lignin qualities, apart from focusing on optimization of reaction conditions and catalyst selection.
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影响因子：
7.5
作者：
T. Yoshikawa;T. Yagi;S. Shinohara;T. Fukunaga;Y. Nakasaka;T. Tago;T. Masuda
通讯作者：
T. Yoshikawa;T. Yagi;S. Shinohara;T. Fukunaga;Y. Nakasaka;T. Tago;T. Masuda
影响因子：
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作者：
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影响因子：
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作者：
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通讯作者：
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影响因子：
2
作者：
Nakamura, Takeshi;Kawamoto, Haruo;Saka, Shiro
通讯作者：
Saka, Shiro