内在矿物对高灰褐煤CO_2气化的影响研究  

Influence of inherent minerals on CO_2 gasification of a lignite with high ash content

作　　者：李昌伦[1] 王永刚[1] 林雄超[1] 田震[1] 武欣[1] 杨远平[1] 张海永[1] 许德平[1] 

机构地区：[1]中国矿业大学(北京)化学与环境工程学院,北京100083

出　　处：《燃料化学学报》2017年第7期780-788,共9页Journal of Fuel Chemistry and Technology

基　　金：国家自然科学基金(21406261);国家科技支撑计划项目(2012BAA04B02)资助~~

摘　　要：利用分选结合逐级酸洗的方法制备出不同灰含量和矿物组成的褐煤煤样,使用沉降管反应器(DTR)和热重分析仪(TGA)研究内在矿物在1 000-1 200℃对褐煤CO_2气化的影响。结果表明,内在矿物对褐煤CO_2气化具有促进作用,且促进机制具有温度敏感性。低温时(1 000℃),内在矿物可通过增加初生半焦微晶结构的无序度,间接提高气化碳转化率。高温时(1 100-1 200℃),内在矿物通过催化煤焦气化,直接促进气化碳转化率的上升。碱性指数不适用于表征本研究的褐煤内在矿物的催化作用。Ca是内在矿物中影响整体催化能力的主要成分,而且羧酸盐形式的Ca是其中的活性组分。不同的催化机制是导致煤焦中钙的催化活性因其化学形式而异的根本原因。羧酸盐形式的Ca可降低煤焦气化反应的活化能,而CaO则提高反应的表观频率因子。Lignite samples with different ash contents and mineral composition were prepared by dry separation and acid washing. A drop tube reactor and thermogravimetric analyzer were used to study effect of inherent minerals on CO2 gasification reaction of lignite at 1 000-1 200 ℃. The results show that the inherent minerals have positive effects on gasification, which are temperature sensitive. At lower gasification temperature（ 1 000 ℃） the inherent minerals can improve carbon conversion indirectly by obstructing the carbon structure order of nascent char. At higher temperatures（ 1 100-1 200 ℃） the inherent minerals can improve carbon conversion by catalyzing nascent char gasification directly. The alkaline index is not suitable for characterizing role of the inherent minerals of lignite in this case. Ca leads to the difference in catalytic activity of the inherent minerals where the most active form is carboxylate. Various catalytic mechanisms are the root cause of different catalytic activity of Ca in different chemical forms. Ca in the form of carboxylate can reduce the activation energy of coal/char gasification reaction,while CaO only promotes the apparent frequency factor.

关 键 词：褐煤 内在矿物 CO2气化 催化机理 化学形式 

分 类 号：TQ541[化学工程—煤化学工程]