强化碳酸化反应体系相平衡基础研究
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摘要
我国是二氧化碳气体（CO_2）排放大国，建立适合我国国情的低成本、低环境风险CO_2减排技术体系，是解决我国温室气体CO_2排放问题的迫切需求，也是世界范围内CO_2减排技术的科技前沿。利用含钙、镁的固体废弃物通过碳酸化反应固定CO_2，在实现了多点源排放CO_2就地加工封存的同时，又实现了固体废弃物的资源化利用，对发展可持续的环保经济具有重要意义。针对利用钢铁渣碳酸化固定CO_2联产碳酸盐产品新工艺应用前景广泛，理论深度不够，理论基础数据缺乏等现状。本文开展了如下研究：
(1)基于强化碳酸化反应体系的主要平衡方程和多元电解质Pitzer模型，初步建立了多相复合溶剂新体系中各主要组分离子活度系数预测模型和碳酸化反应结晶转化率模型。测定了多相复合溶剂新体系中乙酸分配系数，并考察了初始乙酸、乙酸钙浓度以及体系温度对乙酸分配系数的影响。
(2)根据相关文献报道，选取了较为精准的恒定容积法进行高压气液平衡体系中CO_2气体溶解度的计算。设计并搭建完成一套可用于测定高压多相气液相平衡体系中气体溶解度的实验装置，并对实验装置可靠性进行验证，其平均相对偏差为1.62%，可满足实验需求。
(3)对CO_2在磷酸三丁酯中的溶解行为开展了详细研究，并初步研究了CO_2在含钙水溶液中溶解度。测定了温度303.5～363.8K、压力0.5～4.5MPa范围内，CO_2在磷酸三丁酯中的溶解度，并通过GC/MS及FT-IR分析表明，气体以分子形式溶解在TBP溶剂中，CO_2气体在TBP中溶解过程主要为物理吸收，CO_2在TBP中溶解行为与亨利定律基本符合。CO_2在氯化钙中溶解度符合亨利定律，为物理过程，随着氯化钙溶度的增加，CO_2溶解度逐渐增加。
Owing to the large number of CO_2emission in the world, development ofa low cost and low environmental risk technical system for CO_2mitigation isnot only the impending science and technology needs for reducing CO_2emission in China, but also the frontier science and technology of CO_2emission control technology all over the word. Using calcium/magnesiumcontained solid residua as raw materials; CO_2can be sequestrated by indirectmineral carbonation. It can be realized that not only the CO_2can be processedon-site into a solid, but also the solid residua can be utilized as resources,which has important significance on the development of circular economy inChina. Currently, the process of indirect CO_2mineral sequestration withsteel-making slag and carbonate production has a wide application prospect,but lack of theoretical data. The purpose of this paper is to solve theseproblems and the following studies have been done.
(1) In strengthen carbonation reaction system, large number of acetic aciddistribution coefficients were measured, the ionic activity coefficient model ofthe main component and the crystallization conversion rate model ofcarbonation reaction was established.
(2) According to the considerably related literature reports, the preciseconstant volume method was selected to calculate the CO_2solubility in thehigh-pressure multiphase gas-liquid equilibrium system. A set of preciseexperimental apparatus was builded to measure gas solubility data in thehigh-pressure multiphase gas-liquid equilibrium system and the experimentaldevice was proved to be reliable. The average deviation of the experimentaldevice is1.62%and it is enough to meet the experimental demands.
(3) A detailed study on dissolution behavior of CO_2in tributyl-phosphatesolvent and a preliminary study on the solubility of CO_2in solution containingcalcium were implemented. The solubility of CO_2in tributyl phosphate (TBP)solvent was measured in a temperature range of303.15K-363.15K and gaspressure of CO_2up to4.5MPa. Results showed that the solubility of CO_2inTBP solvent increased with the augment of CO_2gas pressure and decreasedwith the growth of equilibrium temperature. GC/MS and FT-IR analysis resultindicated that the capture process by TBP solvent could be regarded asphysical absorption. The Henry coefficient which was obtained by fitting theexperimental data was well consistent with the Henry's law.
(1)基于强化碳酸化反应体系的主要平衡方程和多元电解质Pitzer模型，初步建立了多相复合溶剂新体系中各主要组分离子活度系数预测模型和碳酸化反应结晶转化率模型。测定了多相复合溶剂新体系中乙酸分配系数，并考察了初始乙酸、乙酸钙浓度以及体系温度对乙酸分配系数的影响。
(2)根据相关文献报道，选取了较为精准的恒定容积法进行高压气液平衡体系中CO_2气体溶解度的计算。设计并搭建完成一套可用于测定高压多相气液相平衡体系中气体溶解度的实验装置，并对实验装置可靠性进行验证，其平均相对偏差为1.62%，可满足实验需求。
(3)对CO_2在磷酸三丁酯中的溶解行为开展了详细研究，并初步研究了CO_2在含钙水溶液中溶解度。测定了温度303.5～363.8K、压力0.5～4.5MPa范围内，CO_2在磷酸三丁酯中的溶解度，并通过GC/MS及FT-IR分析表明，气体以分子形式溶解在TBP溶剂中，CO_2气体在TBP中溶解过程主要为物理吸收，CO_2在TBP中溶解行为与亨利定律基本符合。CO_2在氯化钙中溶解度符合亨利定律，为物理过程，随着氯化钙溶度的增加，CO_2溶解度逐渐增加。
Owing to the large number of CO_2emission in the world, development ofa low cost and low environmental risk technical system for CO_2mitigation isnot only the impending science and technology needs for reducing CO_2emission in China, but also the frontier science and technology of CO_2emission control technology all over the word. Using calcium/magnesiumcontained solid residua as raw materials; CO_2can be sequestrated by indirectmineral carbonation. It can be realized that not only the CO_2can be processedon-site into a solid, but also the solid residua can be utilized as resources,which has important significance on the development of circular economy inChina. Currently, the process of indirect CO_2mineral sequestration withsteel-making slag and carbonate production has a wide application prospect,but lack of theoretical data. The purpose of this paper is to solve theseproblems and the following studies have been done.
(1) In strengthen carbonation reaction system, large number of acetic aciddistribution coefficients were measured, the ionic activity coefficient model ofthe main component and the crystallization conversion rate model ofcarbonation reaction was established.
(2) According to the considerably related literature reports, the preciseconstant volume method was selected to calculate the CO_2solubility in thehigh-pressure multiphase gas-liquid equilibrium system. A set of preciseexperimental apparatus was builded to measure gas solubility data in thehigh-pressure multiphase gas-liquid equilibrium system and the experimentaldevice was proved to be reliable. The average deviation of the experimentaldevice is1.62%and it is enough to meet the experimental demands.
(3) A detailed study on dissolution behavior of CO_2in tributyl-phosphatesolvent and a preliminary study on the solubility of CO_2in solution containingcalcium were implemented. The solubility of CO_2in tributyl phosphate (TBP)solvent was measured in a temperature range of303.15K-363.15K and gaspressure of CO_2up to4.5MPa. Results showed that the solubility of CO_2inTBP solvent increased with the augment of CO_2gas pressure and decreasedwith the growth of equilibrium temperature. GC/MS and FT-IR analysis resultindicated that the capture process by TBP solvent could be regarded asphysical absorption. The Henry coefficient which was obtained by fitting theexperimental data was well consistent with the Henry's law.
引文
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