离子液体催化热解纤维素制备左旋葡萄糖酮的研究  

Levoglucosenone production by catalytic pyrolysis of cellulose using ionic liquid as catalyst

作　　者：徐安邦 黄鑫[1] 冉景煜[1] 唐广川 杨仲卿[1] 秦昌雷[1] 曹景沛[2] XU An-bang;HUANG Xin;RAN Jing-yu;TANG Guang-chuan;YANG Zhong-qing;QIN Chang-lei;CAO Jing-pei(Key Laboratory of Low-grade Energy Utilization Technologies&Systems,Ministry of Education,Chongqing University,Chongqing 400044,China;Key Laboratory of Coal Processing and Efficient Utilization,Ministry of Education,China University of Mining and Technology,Xuzhou 221116,China)

机构地区：[1]重庆大学低品位能源利用技术及系统教育部重点实验室,重庆400044 [2]中国矿业大学煤炭深加工与洁净利用教育部重点实验室,江苏徐州221116

出　　处：《燃料化学学报》2022年第6期768-776,共9页Journal of Fuel Chemistry and Technology

基　　金：国家自然科学基金(52006019);中国博士后科学基金(2020M673132);重庆市自然科学基金(cstc2020jcyj-bshX0099)资助。

摘　　要：纤维素是世界上含量最丰富的可再生有机碳资源之一,左旋葡萄糖酮(LGO)是来源于纤维素热解的一种高附加值平台化合物。本研究考察了离子液体烷基侧链长度对纤维素催化热解制备LGO的影响规律。实验结果表明,最短侧链的1-丁基-2,3-二甲基三氟甲烷磺酸咪唑离子液体对LGO表现了最好的催化效果,其原因是侧链长度减少导致离子液体阴阳离子间相互作用减弱,使离子液体扩散增强。在300℃热解时LGO产率达到15.6%-C,离子液体的回收率为95.9%,其重复利用三次后LGO的产率只有轻微下降。通过密度泛函理论得到了LGO的最佳生成路径,其最低反应活化能为176.2 kJ/mol。此外,本方法也可同时获得多孔性的焦炭,其最高比表面积和孔容分别为389.4 m^(2)/g和0.689 cm^(3)/g。Cellulose is one of the most abundant renewable organic carbon resources in the world.Levoglucosenone(LGO)is a high value-added platform chemical derived from cellulose pyrolysis.In this study,the influence of ionic liquid catalyst on the production of LGO by catalytic pyrolysis of cellulose was revealed.The results showed that 1-butyl-2,3-dimethylimidazolium triflate performed best for the LGO formation.The reason was that the decrease in the length of the side chain weakened the interaction between the cation and anion of the ionic liquid,which increased the diffusion of the ionic liquid.LGO reached a yield of 15.6%-C at pyrolysis temperature of 300℃,and the recovery rate of ionic liquid attained to 95.9%.Besides,LGO yield only slightly decreased after 3 times re-utilization of the ionic liquid.The formation path of LGO was calculated by density functional theory.The result showed the lowest activation energy was 176.2 kJ/mol.Moreover,this method was effective to obtain porous char at the same time,and the highest specific surface area and pore volume were 389.4 m^(2)/g and 0.689 cm^(3)/g,respectively.

关 键 词：纤维素 离子液体 热解 左旋葡萄糖酮 多孔性焦炭 

分 类 号：TQ028.8[化学工程]