| 强化碳酸化固定CO2反应过程分析与机理探讨 |
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| 引用本文： | 包炜军,李会泉,张懿. 强化碳酸化固定CO2反应过程分析与机理探讨[J]. 化工学报, 2009, 60(9): 2332 |
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| 作者姓名： | 包炜军 李会泉 张懿 |
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| 作者单位： | 中国科学院过程工程研究所，湿法冶金清洁生产技术国家工程实验室; 中国科学院研究生院 |
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| 基金项目： | 国家科技支撑计划，国家重点基础研究发展规划(973计划) |
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| 摘 要： | 以乙酸为媒质的间接碳酸化固定CO2工艺路线，主要包括乙酸媒质浸出钙镁离子形成乙酸盐，碳酸化过程乙酸盐转化成碳酸钙产品，同时生成乙酸媒质循环利用。然而在碳酸化过程碳酸化反应结晶转化率低，从而制约该工艺路线的进一步工业应用。采用有机溶剂TBP萃取乙酸与碳酸钙结晶过程耦合，可以实现碳酸化反应结晶转化率的大幅度提高。通过实验研究了体系达到平衡时初始乙酸钙浓度对碳酸化过程的影响，结果表明碳酸化反应结晶转化率都在40%以上，比文献报道的高出一倍。基于强化碳酸化过程的机理分析，初步进行了耦合过程的热力学平衡计算。研究结果表明：由于有机溶剂TBP的加入，体系的酸性条件得到改善，有利于碳酸钙结晶析出；然而高浓度条件下，乙酸根与钙离子之间强烈的相互作用成为进一步提高碳酸化反应结晶转化率的主要障碍。
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| 关 键 词： | 二氧化碳 矿物碳酸化 反应结晶 过程强化 |
Process analysis and mechanism discussion of enhanced CO2 sequestration by mineral carbonation |
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| BAO Weijun,LI Huiquan,ZHANG Yi. Process analysis and mechanism discussion of enhanced CO2 sequestration by mineral carbonation[J]. Journal of Chemical Industry and Engineering(China), 2009, 60(9): 2332 |
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| Authors: | BAO Weijun LI Huiquan ZHANG Yi |
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| Abstract: | Indirect CO2 mineral sequestration that involves two separate steps, with acetic acid as the recycling medium, was limited by a crystallization conversion of only 20% in the second gas-liquid reactive crystallization step.In this paper, the second carbonation step was greatly improved by coupling reactive crystallization and solvent extraction with the introduction of an organic solvent, tributyl phosphate (TBP), to the process.The effect of the initial concentration of calcium acetate in the aqueous solution on the crystallization conversion was studied experimentally.The obtained calcium conversion was above 40%, which was one time higher than that reported in the literature.Based on the mechanism discussion and thermodynamic equilibrium calculation analysis, it can be concluded that adding TBP to the step can consume the produced acetic acid, and it is in favor of the precipitation of calcium carbonate.While the challenge presented by the strong interaction between calcium ions and acetate ions for further improving crystallization conversion cannot be solved only by the addition of TBP. |
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