纤维素分子在跨相表界面体系中的定向催化转化机理研究

批准号:
21978249
项目类别:
面上项目
资助金额:
65.0 万元
负责人:
刘健
依托单位:
学科分类:
生物质转化与轻工制造
结题年份:
2023
批准年份:
2019
项目状态:
已结题
项目参与者:
刘健
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中文摘要
纤维素是自然界最丰富的生物质,其β-1,4-苷键裂解后可以制造各类化学品,有希望替代传统化石能源。高效定向水解转化技术是纤维素能源化利用的关键,但传统技术存在着反馈抑制和副反应难以调控的问题。前期研究表明,利用萃取技术和热力学平衡原理建立包含非极性相和水相的相界面水解体系可以克服上述问题,但其机理尚不清楚。本研究将利用分子模拟手段探明纤维素在水相和非极性相的相界面环境中石墨烯基磺酸催化下局域原子和电子结构,探讨苷键在这一特殊体系中的断裂规律,剖析纤维素分子在相界面环境体系中电子传递的机理,衡量相界面体系对反应活化能的影响,并针对内外切混合和逐级外切两种苷键催化模式分别建模分析,基于反应动力学原理总结纤维素的各级降解过程中反应活化能的变化规律,以及纤维素分子在相界面的选择活化和可控重构机理,剖析纤维素苷键在相界面体系中断裂的影响因素,从分子水平认识该过程,为提高转化效率提供理论依据。
英文摘要
As the most popular biomass, cellulose has gained a lot of interest because of many technological and energy benefits and lots of research are going on to explore their substitution to traditional fossil fuel. The successful controllable hydrolysis technology of cellulose is of great importance to produce biofuel. However, the existing technologies have the limitation of either inhibited by products or over-reaction. In preliminary research, a new process for cellulose hydrolysis that combines hydrolysis and product separation is proposed, form a liquid-solid-liquid three-phase system that contains solid cellulose, non-polar liquid and water phase, so that the issues of inhibition and over-reaction can be solved. It was based on the principles of thermodynamic equilibrium and extraction, but the mechanism is unclear. This research attempts to ascertain the distribution coefficient of local atom and electron structure in the phase interface, chemical composition of reactant and degree of crystalline in the phase interface hydrolysis process will be investigated with a series of molecular simulation and experimental methods. The transformation of cellulose to cello-oligosaccharide and glucose can be better understood by simulating and measuring the glycosidic bonds distribution of sugars. The reaction mechanism to reduce the activation energy in hydrolysis process will be focused in this study by the analysis of endo- and exo- avtivities of cutting glycosidic bonds through modeling and validation. The variation of activation energy with the progress of cellulose hydrolysis to glucose and HMF will be explored based on the reaction kinetics in the phase interface system. This study could will provide a theoretical basis for scientific understanding of the reaction process and build a new liquid-solid-liquid three-phase system of cellulose hydrolysis to achieve higher glucose yields. The regulation mechanism for catalytic hydrolysis to get high yield of biofuel will be developed based on the above work. The influence of various parameters on the yield and selectivity will be quantified, so that the compositions of glucose and cello-oligosaccharide in the products can be controlled. Thus scientific understanding the process and provide theoretical basis for improving the efficiency of reaction is realized.
期刊论文列表
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专利列表
DOI:10.1016/j.carbon.2019.11.065
发表时间:2020-03-01
期刊:CARBON
影响因子:10.9
作者:Long, Sishi;Feng, Yunchao;Long, Minnan
通讯作者:Long, Minnan
DOI:10.6043/j.issn.0438-0479.202002028
发表时间:2021
期刊:厦门大学学报. 自然科学版
影响因子:--
作者:和帅帅;刘健;龚正良;甘礼惠;龙敏南
通讯作者:龙敏南
DOI:10.6043/j.issn.0438-0479.202003066
发表时间:2021
期刊:厦门大学学报. 自然科学版
影响因子:--
作者:洪华驰;刘健;甘礼惠;龙敏南
通讯作者:龙敏南
DOI:https://doi.org/10.1016/j.nanoen.2021.105973
发表时间:2021
期刊:Nano Energy
影响因子:17.6
作者:Sishi Long;Yunchao Feng;Faliang He;Jizhong Zhao;Tian Bai;Hongbin Lin;Wanli Cai;Chaowu Mao;Yuhan Chen;Lihui Gan;Jian Liu;Meidan Ye;Xianhai Zeng;Minnan Long
通讯作者:Minnan Long
DOI:10.1016/j.eurpolymj.2020.109651
发表时间:2020-04
期刊:European Polymer Journal
影响因子:6
作者:Moshuqi Zhu;Jian Liu;L. Gan;M. Long
通讯作者:Moshuqi Zhu;Jian Liu;L. Gan;M. Long
纤维素三相水解机理的研究
- 批准号:21303142
- 项目类别:青年科学基金项目
- 资助金额:25.0万元
- 批准年份:2013
- 负责人:刘健
- 依托单位:
国内基金
海外基金
