CIESC Journal ›› 2010, Vol. 61 ›› Issue (10): 2579-2584.

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Mechanism and kinetics of cellobiose hydrogenation catalyzed by Ru/CNT

TAN Xuesong;ZHUANG Xinshu;DENG Weiping;ZHANG Qinghong;WANG Ye;YUAN Zhenhong   

  • Online:2010-10-05 Published:2010-10-05

Ru/CNT催化纤维二糖加氢制备山梨醇的机理及动力学

谭雪松;庄新姝;邓卫平;张庆红;王野;袁振宏   

  1. 中国科学院广州能源研究所,中国科学院可再生能源与天然气水合物重点实验室;厦门大学化学化工学院化学系,固体表面物理化学国家重点实验室,醇醚酯国家工程实验室

Abstract:

The production of chemicals or fuels from renewable biomass resources especially cellulose has attracted much attention because of the worldwide demand for less dependence on fossil resources. However, the direct utilization of cellulose is still a challenge because of its robust crystalline structure.Herein,the hydrogenation of cellobiose,a typical cellulose, over carbon nanotube supported ruthenium catalyst (Ru/CNT) was reported.The mechanism of cellobiose conversion was proposed and the kinetic equation was obtained.Based on the kinetic experiments carried out in the range 120—185℃ under 5.0 MPa H2, the reaction rate constants and activation energies of each reaction step in cellobiose hydrogenation were obtained with MATLAB, in which the activation energy for hydrolysis and hydrogenolysis of cellobiose was estimated as 147.1 kJ·mol-1 and 71.2 kJ·mol-1, respectively.The obtained kinetic model and some general rules on the catalytic hydrogenation of cellobiose may provide important data for efficient utilization of cellulose.

Key words: 钌, 碳纳米管, 纤维二糖, 催化加氢, 机理, 动力学

摘要: 针对纤维素的转化,研究了以钌碳纳米管(Ru/CNT)为催化剂,纤维素模型分子纤维二糖催化加氢制备山梨醇的反应。通过对反应产物的分析,考察了纤维二糖转化生成山梨醇的反应机理,建立了纤维二糖催化加氢的动力学模型。并根据实验数据,拟合得到纤维二糖催化加氢反应各步的反应数率常数和表观活化能,其中,纤维二糖水解活化能为147.1 KJ·mol-1;纤维二糖部分加氢活化能为73.8 KJ·mol-1。纤维二糖催化加氢反应模型的建立,为纤维素资源的高效利用提供了重要的基础数据。

关键词: 钌, 碳纳米管, 纤维二糖, 催化加氢, 机理, 动力学