洁净煤技术

2021, v.27;No.132(02) 180-186

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不同钙基吸附剂捕集CO_2后的硫酸化反应特性研究
Study on sulfation reaction characteristics of different calcium-based sorbents after CO_2 capture

孙锋;申成;罗聪;罗童;
SUN Feng;SHEN Cheng;LUO Cong;LUO Tong;China Ship Development and Design Center;State Key Laboratory of Coal Combustion,Huazhong University of Science and Technology;

摘要(Abstract):

钙基吸附剂进行多次CO_2捕集后,碳酸化效率会大幅衰减,此时的吸附剂能否高效脱硫利用是值得重点关注的问题。鉴于此,筛选了高性能合成钙基吸附剂和天然石灰石吸附剂,通过热重分析仪分析对比其在多循环CO_2捕集后的碳酸化和硫酸化反应性能,采用微粒模型研究其硫酸化反应动力学特征。结果发现,高性能合成钙基吸附剂的碳酸化反应速率和CO_2吸附能力明显高于石灰石吸附剂。在长达500循环的CO_2捕集试验后,高性能合成钙基吸附剂的CO_2吸附能力比石灰石高10倍以上,其SO_2吸附能力相较于石灰石提升约40%。经历多次CO_2捕集反应循环后,2种吸附剂的硫酸化能力均有提升:其中,石灰石吸附剂的提升幅度更大,硫酸化转化率从26%提升到35%,而高性能合成钙基吸附剂的硫酸化转化率则从38%提升到43%。通过微粒模型计算发现,2种吸附剂的硫酸化反应均是与SO_2浓度相关的一级反应,多循环捕集CO_2反应后,石灰石吸附剂的硫酸化反应活化能下降接近30%,而高性能合成钙基吸附剂的硫酸化反应活化能只下降了5%。研究结果说明2种不同钙基吸附剂在进行循环CO_2捕集后,脱硫能力得到了不同程度的提高,且均可以较好地应用于SO_2的脱除。
The carbonation conversion of the calcium-based sorbent decreases significantly after multiple CO_2 capture cycles,whether the sorbent can be further used efficiently in desulfurization reaction is important issue which deserves concerns. In order to delve into this issue,the high performance calcium-based sorbent and natural limestone sorbent were selected,the carbonation and sulfation reaction performance after multiple CO_2 capture cycles were analyzed and compared by thermal gravimetric analyzer,and the sulfation kinetics characteristics were studied by particle model. The results showed that the rate of carbonation reaction and CO_2 adsorption capacity of the high performance calcium-based sorbents are much higher than those of limestone adsorbent. After multiple cycles of CO_2 capture test,the CO_2 adsorption capacity of high performance calcium-based sorbents is over 10 times higher than that of limestone,and its SO_2 adsorption capacities was improved by 40% than that of limestone. After multiple CO_2 capture reactions,their sulfation abilities are both improved. The improvement of limestone is greater,the sulfation conversion is increased from 26% to 35%,while the sulfation conversion of high performance calcium-based sorbent is increased from 38% to 43%. It is found through particle model calculation that the sulfation process of both sorbents is a first-order reaction related to the concentration of SO_2. After the multiple CO_2 capture cycles,the activation energy of sulfation reaction of limestone decreases by nearly 30%,while that of high performance calcium-based sorbent only decreases by 5%. The results indicate that the desulphurization capacity of two different calcium-based sorbents can be improved to different degrees after multiple CO_2 capture cycles,and both of them can be better used for SO_2 removal.

关键词(KeyWords): 钙基吸附剂;硫酸化;CO_2捕集;微粒模型;反应动力学
calcium-based sorbents;sulfation;CO_2 capture;particle model;reaction kinetics

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基金项目(Foundation): 国家自然科学基金资助项目(51606076)

作者(Author): 孙锋;申成;罗聪;罗童;
SUN Feng;SHEN Cheng;LUO Cong;LUO Tong;China Ship Development and Design Center;State Key Laboratory of Coal Combustion,Huazhong University of Science and Technology;

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DOI: 10.13226/j.issn.1006-6772.CCUS20092001

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