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Reversible covalent chemistry of carbon dioxide unlocks the recalcitrance of cellulose for its enzymatic saccharification
Bioresource Technology ( IF 9.7 ) Pub Date : 2019-10-03 , DOI: 10.1016/j.biortech.2019.122230
Jianyun Gan , Ya Peng , Qin Chen , Gang Hu , Qinqin Xu , Longming Jin , Haibo Xie

To overcoming the natural recalcitrance of cellulose for glucose production via enzymatic hydrolysis, a new strategy of destroying hydrogen bond donor to reconstruct cellulose’s hydrogen bonding network was developed via a mild reversible reaction of cellulose with CO2 catalyzed by organic bases. The reaction dynamics of cellulose with CO2 in the presence of organic bases was studied by using in situ IR. Investigation also included how the organic bases in pretreatment media and pretreatment parameters including CO2 pressure, pretreatment temperature and time affected the physical-chemical structure of cellulose by Fourier Transform Infrared Spectroscopy (FT-IR), X-ray diffraction (XRD), scanning electron microscopy (SEM) and Atomic force microscopy (AFM) and subsequent enzymatic scarification of cellulose. The findings showed that dissolution activation efficiency significantly correlated to various parameters, that can be optimized to be the tetramethyl guanidine (TMG)/CO2/DMSO solvent system at 50 oC, 2 MPa of CO2 for 2 h, by which a complete transformation the cellulose crystalline structure from I to II, and 100% glucose yield were achieved. The recyclability and usability are also investigated.



中文翻译:

二氧化碳的可逆共价化学解开了纤维素酶促糖化的顽固性

为了克服纤维素通过酶促水解生产葡萄糖的天然顽抗性,通过纤维素与有机碱催化的CO 2的温和可逆反应,开发了一种破坏氢键供体以重建纤维素氢键网络的新策略。通过使用原位红外光谱研究了纤维素在有机碱存在下与CO 2的反应动力学。调查还包括预处理介质中的有机碱以及包括CO 2在内的预处理参数压力,预处理温度和时间通过傅立叶变换红外光谱(FT-IR),X射线衍射(XRD),扫描电子显微镜(SEM)和原子力显微镜(AFM)以及随后的酶促酶解作用影响了纤维素的物理化学结构纤维素。研究结果表明,溶解活化效率与各种参数显着相关,可以将其优化为四甲基胍(TMG)/ CO 2 / DMSO溶剂体系,温度为50 o C,2 MPa的CO 2持续2 h,从而完成将纤维素的晶体结构从I转变为II,并实现了100%的葡萄糖收率。还研究了可回收性和可用性。

更新日期:2019-10-03
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