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在高固含量下,酶水解受生物质与水相互作用的限制:通过底物修饰提高性能。

Enzymatic hydrolysis is limited by biomass-water interactions at high-solids: improved performance through substrate modifications.

作者信息

Weiss Noah D, Felby Claus, Thygesen Lisbeth G

机构信息

Department of Geosciences and Natural Resource Management, University of Copenhagen, Frederiksberg, Denmark.

出版信息

Biotechnol Biofuels. 2019 Jan 4;12:3. doi: 10.1186/s13068-018-1339-x. eCollection 2019.

Abstract

BACKGROUND

To improve process economics for production of fuels and chemicals from lignocellulosic biomass, high solids concentrations are applied in enzymatic hydrolysis, to increase product concentration and reduce energy input. However, increasing solids concentrations decrease cellulose conversion yields, the so called 'high-solids effect.' Previous work suggests that product inhibition and mixing contribute, but an understanding of how biomass properties influence the high-solids effect, is lacking.

RESULTS

Cellulose hydrolysis yields with an industrial cellulase (Ctec2) were measured on pretreated wheat straw and spruce from 5 to 30% dry matter (DM), and compared to yields of an older industrial cellulase mixture (Celluclast 1.5L/Novozym188). For Ctec2, yield was independent of DM below 15-18% DM, while yields decreased with increasing DM above this range, but at different rates for each biomass. For Celluclast 1.5L/Novozym188, yields decreased already from the lowest DM, suggesting that the high-solids effect was more a function of product inhibition, while the yields of the newer Ctec2 mixture were driven more by biomass-water interactions. LF-NMR relaxometry showed that the onset of the high-solids effect for Ctec2 corresponded to the disappearance of free water from the system, and a decrease in water self-diffusion rates. While the spruce had higher yields at low-solids, the wheat straw had higher yields at high-solids conditions, exhibiting that relative yields at low and high-solids are not related. Higher yields corresponded to increased water constraint by the biomass at high-solids conditions. Modifications to the pretreated wheat straw resulted in improved yields, and changes to the inflection point and intensity of the high-solids effect, showing that this effect can be reduced.

CONCLUSIONS

The high-solids effect is both enzyme and substrate dependent, and can be reduced by modifying the pretreated biomass, suggesting that pretreatment processes can be designed to achieve similar effects. Yields at low and high-solids concentrations do not correlate for a given biomass, and thus industrial evaluation of biomass recalcitrance should be carried out at high-solids conditions.

摘要

背景

为了提高从木质纤维素生物质生产燃料和化学品的工艺经济性,在酶水解过程中采用高固含量,以提高产物浓度并减少能量输入。然而,固含量的增加会降低纤维素转化率,即所谓的“高固含量效应”。先前的研究表明,产物抑制和混合是造成这种现象的原因,但对于生物质特性如何影响高固含量效应仍缺乏了解。

结果

使用一种工业纤维素酶(Ctec2),在预处理后的小麦秸秆和云杉上测定了5%至30%干物质(DM)含量下的纤维素水解产率,并与一种较老的工业纤维素酶混合物(Celluclast 1.5L/Novozym188)的产率进行了比较。对于Ctec2,在干物质含量低于15 - 18%时,产率与干物质含量无关,而在此范围之上,产率随干物质含量增加而下降,但每种生物质下降的速率不同。对于Celluclast 1.5L/Novozym188,从最低干物质含量时产率就开始下降,这表明高固含量效应更多是产物抑制的作用,而新型Ctec2混合物的产率更多是由生物质 - 水相互作用驱动的。低场核磁共振弛豫测量表明,Ctec2的高固含量效应的起始点对应于体系中自由水的消失以及水自扩散速率的降低。虽然云杉在低固含量时有较高产率,但小麦秸秆在高固含量条件下有较高产率,这表明低固含量和高固含量时相对产率并无关联。较高产率对应于高固含量条件下生物质对水约束的增加。对预处理后的小麦秸秆进行改性可提高产率,并改变高固含量效应的拐点和强度,表明这种效应可以降低。

结论

高固含量效应既依赖于酶也依赖于底物,并且可以通过对预处理后的生物质进行改性来降低,这表明预处理工艺可以设计成达到类似效果。对于给定的生物质,低固含量和高固含量时的产率并无关联,因此对生物质抗降解性的工业评估应在高固含量条件下进行。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3bd4/6318902/305b34a4f1de/13068_2018_1339_Fig1_HTML.jpg

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