煤液化铁基催化剂对煤焦气化特性影响和动力学研究  

Effect of iron-based catalyst from coal liquefaction on coal char gasification reactivity and kinetics

作　　者：何清 李恒 王思敏 程晨 郭庆华[1,2] 于广锁 HE Qing;LI Heng;WANG Si-min;CHENG Chen;GUO Qing-hua;YU Guang-suo(Institute of Clean Coal Technology,East China University of Science and Technology,Shanghai 200237,China;State Key Laboratory of High-efficiency Coal Utilization and Green Chemical Engineering,Ningxia University,Yinchuan 750021,China)

机构地区：[1]华东理工大学洁净煤技术研究所,上海200237 [2]宁夏大学省部共建煤炭高效利用与绿色化工国家重点实验室,宁夏银川750021

出　　处：《燃料化学学报》2022年第2期143-151,共9页Journal of Fuel Chemistry and Technology

基　　金：国家重点研发计划(2017YFB0602404)资助。

摘　　要：本研究以哈密原煤和脱矿煤为原料,研究煤液化铁基催化剂对煤焦结构和气化反应性的影响。利用扫描电镜能谱仪和物理吸附仪研究煤焦表面形貌、元素分布和介孔特性,利用热重分析仪研究煤焦气化特性,采用model-fitting和model-free方法研究反应动力学。结果表明,脱矿和负载催化剂对煤焦表面附着物的影响较主体基质明显。负载催化剂的煤焦比表面积显著增加。铁基催化剂提升煤焦气化活性可归因于煤焦表面富集较多Fe和AAEMs等元素,以及比表面积的增大。负载催化剂的脱矿煤焦表现出较大的相对催化活性,且其对升温速率和碳转化率的变化不敏感。煤焦气化特性的差异将随升温速率的升高而减小。铁基催化剂可提高原煤焦的气化反应指前因子A,降低脱矿煤焦的反应活化能E_(a)。非等温条件下,煤焦气化反应活化能随转化率的增加而降低。根据模型拟合度和动力学补偿效应,随机孔模型是描述煤焦气化的最佳模型,且更适合于脱矿煤焦(催化)气化。In the present work,the effects of iron-based catalysts from coal liquefaction on the coal structure and gasification reactivity were studied using the Hami raw coal and demineralized coal.The surface morphology,element distribution and mesoporous characteristics of coal char were investigated by SEM-EDS and physical adsorption analyzer.The gasification reactivity was performed in a thermogravimetric analyzer.The gasification kinetics was studied through the model-fitting and model-free methods.The results showed that the demineralization and catalyst loading had more obvious effect on the surface attachments than the carbon matrix.The coal char with catalyst loading had significant larger specific surface area(SSA).The reactivity improvement by iron-based catalyst was attributed to the enrichment of Fe and AAEMS and increase of SSA for coal char.More pronounced relative catalytic activity was observed for the catalytic gasification of demineralized coal char,and its activity was not sensitive to the change of heating rate and carbon conversion.The gasification characteristics difference decreased with the increase of heating rate.The iron-based catalyst increased the pre-exponential factor A for the demineralized coal char gasification,and reduced the activation energy E_(a) for the raw coal char gasification.Under the non-isothermal conditions,the E_(a) decreased with conversion.According to fitting performance and kinetic compensation effect,the random pore model was the best model to describe gasification,especially for the(catalytic)gasification of the demineralized coal char.

关 键 词：煤气化 动力学 铁基催化剂 催化气化 脱矿 

分 类 号：TQ530.2[化学工程—煤化学工程]