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化工学报  2015 

水蒸气对煅烧石灰石碳酸化反应影响的实验与模型分析

DOI: 10.11949/j.issn.0438-1157.20141419, PP. 1088-1096

Keywords: 二氧化碳捕集,化学反应,催化,产物层扩散系数,活化能

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Abstract:

利用热重分析仪,对比了不同反应温度、不同水蒸气浓度对煅烧石灰石碳酸化反应的影响。碳酸化反应温度在500℃时,反应初期水蒸气对碳酸化反应的影响并不明显,反应10min之后,在含有1.5%、10%和20%(体积分数)水蒸气条件下碳酸化转化率比无水蒸气条件下转化率分别提高了19.8%、27.2%和30.5%。水蒸气的存在有助于提高碳酸化反应转化率,但随着水蒸气浓度的增加转化率增加幅度减小。利用随机孔隙模型,对产物层扩散阶段扩散系数及反应活化能进行了计算。高温条件下,气氛中含有1.5%的水蒸气使反应活化能从237.7kJ·mol-1降低到179.9kJ·mol-1,提高水蒸气浓度到10%和20%后,反应活化能从156.6kJ·mol-1降低到148.6kJ·mol-1。不同水蒸气浓度条件下,碳酸化反应存在两个明显特征:一是大约在550℃处存在一个明显扩散系数的斜率变化,这一温度与气氛中是否存在水蒸气无关;另一特征是随着反应温度的提高,水蒸气的促进作用减弱。依据实验和模型计算结果,推测了当反应处于产物层扩散阶段时水蒸气对碳酸化反应影响的作用机理。

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