Solid-State NMR Studies of Solvent-Mediated, Acid-Catalyzed Woody Biomass Pretreatment for Enzymatic Conversion of Residual Cellulose,ACS Sustainable Chemistry & Engineering

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Solid-State NMR Studies of Solvent-Mediated, Acid-Catalyzed Woody Biomass Pretreatment for Enzymatic Conversion of Residual Cellulose
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2020-04-14 , DOI: 10.1021/acssuschemeng.0c01538
Theodore W Walker _{1,

2} , Nathaniel Kuch _{2,

3} , Kirk A Vander Meulen _{2,

3} , Catherine F M Clewett ₄ , George W Huber ₁ , Brian G Fox _{2,

3} , James A Dumesic _{1,

2}

Affiliation

Enzymes selectively hydrolyze the carbohydrate fractions of lignocellulosic biomass into corresponding sugars, but these processes are limited by low yields and slow catalytic turnovers. Under certain conditions, the rates and yields of enzymatic sugar production can be increased by pretreating biomass using solvents, heat, and dilute acid catalysts. However, the mechanistic details underlying this behavior are not fully elucidated, and designing effective pretreatment strategies remains an empirical challenge. Herein, using a combination of solid-state and high-resolution magic-angle-spinning NMR, infrared spectroscopy, and X-ray diffractometry, we show that the extent to which cellulase enzymes are able to hydrolyze solvent-pretreated biomass can be understood in terms of the ability of the solvent to break the chemical linkages between cellulose and noncellulosic materials in the cell wall. This finding is of general significance to enzymatic biomass conversion research, and implications for designing improved biomass conversion strategies are discussed. These findings demonstrate the utility of solid-state NMR as a tool to elucidate the key chemical and physical changes that occur during the liquid-phase conversion of real biomass.

中文翻译：

用于残留纤维素酶转化的溶剂介导、酸催化木本生物质预处理的固态核磁共振研究

酶选择性地将木质纤维素生物质的碳水化合物部分水解成相应的糖，但这些过程受到低产率和缓慢的催化周转的限制。在某些条件下，可以通过使用溶剂、热和稀酸催化剂预处理生物质来提高酶促糖生产的速率和产量。然而，这种行为背后的机制细节尚未完全阐明，设计有效的预处理策略仍然是一个实证挑战。在此，结合使用固态和高分辨率魔角旋转核磁共振、红外光谱和 X 射线衍射，我们表明纤维素酶能够水解经溶剂预处理的生物质的程度可以理解为溶剂破坏细胞壁中纤维素和非纤维素材料之间的化学键的能力。这一发现对于酶促生物质转化研究具有普遍意义，并讨论了设计改进的生物质转化策略的意义。这些发现证明了固态核磁共振作为一种工具的实用性，可以阐明真实生物质液相转化过程中发生的关键化学和物理变化。

更新日期：2020-04-23

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