随着温室效应的加剧，CO₂利用逐渐成为研究的热点。CO₂资源化转化为碳基化学品对于温室气体的减排、减少碳资源的浪费将至关重要。由于碳酸钙工业在石灰窖煅烧石灰矿阶段产生大量CO₂，造成温室效应和碳资源的浪费。因此，针对窖气CO₂捕集和高附加值利用具有重要的环境和社会效益。本课题选取典型的石灰窖窖气为原料，基于化工流程模拟软件Aspen Plus对石灰窖窖气生产高纯CO₂联产NaHCO₃工艺进行了研究，分步构建了CO₂捕集、高纯CO₂生产、NaHCO₃生产和副产品(NH₄)₂SO₄回收的模型。并对各工序进行分析验证，最终采用耦合的思想进行整合，形成完整的工艺流程模型并对其进行了技术经济分析。

本课题针对以下四个方面展开研究：（1）CO₂捕集采用甲基二乙醇胺（MDEA）吸收-解吸工艺，根据年度总费用（TAC），对吸收塔和解吸塔进行了参数优化，将原料气CO₂提纯到0.9254（摩尔分率，下同），CO₂回收率达到99.45%。但CO₂气体中仍有0.07383的H₂O、1.342×10^-5的CH₄、1.205×10^-6的C₂H₄、1.053×10^-5的CO、5.415×10^-4的N₂和1.566×10^-4的O₂。（2）高纯CO₂生产采用催化燃烧法除去CO₂气体中的可燃物，加压后首先通过汽提塔塔底脱除大量H₂O，然后在精馏塔塔顶脱除轻组分，塔底得到纯度0.99999的CO₂产品，汽提塔塔底和精馏塔塔顶大量未利用的CO₂输送到NaHCO₃生产工序作为原料。为了降低生产能耗，利用夹点技术进行能量分析，通过双效精馏和换热网络实现热集成，回收热量280167.6 kJ/h。（3）NaHCO₃的生产采用硫酸钠碳酸化法，利用廉价易得的钠芒硝、NH₃和CO₂于奥斯陆结晶器内反应得到NaHCO₃晶体。分析了NH₃、Na₂SO₄、温度和压力对结晶器的影响，结果表明，随着NH₃进料流量的增加，有利于CO₂的捕集，但过量的NH₃会产生副产物NH₄HCO₃；CO₂捕集率随芒硝用量增加而增加；过高的结晶温度不利于CO₂的捕集和碳酸氢钠的结晶；压力对反应影响较小。最终确定反应条件，结晶温度为35.5 ℃，常压操作，以氨作为限制反应物，饱和芒硝进料，进料摩尔比Na₂SO₄:CO₂:NH₃= 1.2:2:1。（4）针对副产物Na₂SO₄和(NH₄)₂SO₄混合物，首先探讨了强碱蒸氨法回收氨气，结果表明该方法并不适合。基于溶解度曲线，开发热法重结晶的方式对副产物进行分离，由于缺少相关文献参数，设计蒸发-冷却-冷却方式分离副产物实验，通过实验数据确定模拟过程参数，最终回收尾液中80.32%的硫酸钠，22.31%的硫酸铵。

最后，通过Aspen Process Economic Analyzer V11.0对全流程经济分析可知，本项目于6.45年开始盈利，并且净收益率为14.73%，表明该项目具有一定的经济效益。

With the intensification of the greenhouse effect, CO₂ utilization has gradually become a research hotspot. The conversion of CO₂ resources into carbon-based chemicals will be crucial for reducing greenhouse gas emissions and reducing carbon waste. Due to the large amount of CO₂ generated by the calcium carbonate industry during the lime pit calcination stage, leads to the greenhouse effect and waste of carbon resources. Therefore, the capture and high value-added utilization of CO₂ in cellar gas have important environmental and social benefits. In this paper, the typical lime cellar gas was selected as raw material. Based on the chemical process simulation software Aspen Plus, the process of producing high-purity CO₂ and NaHCO₃ from lime cellar gas was studied. The models of CO₂ capture, high purity CO₂ production, NaHCO₃ production, and by-product (NH₄)₂SO₄ recovery were constructed step by step. Each process is analyzed and verified, and finally, the coupling idea is used to integrate to form a complete process flow model and carry out a technical and economic analysis.

This study focuses on the following four aspects: (1) CO₂ capture using methyl diethanolamine (MDEA) absorption desorption process. Based on the annual total cost (TAC), the parameters of the absorption and desorption towers were optimized. The raw gas CO₂ was purified to 0.9254 (molar fraction, the same as below), and the CO₂ recovery rate reached 99.45%. However, there is still 0.07383 of H₂O, 1.342×10^-5 of CH₄, 1.205×10^-6 of C₂H₄, 1.053×10^-5 of CO, 5.415×10^-4 of N₂, and 11.566×10^-4 of O₂ in the CO₂ gas. (2) The production of high-purity CO₂ uses catalytic combustion to remove combustibles from the CO₂ gas. After pressurization, a large amount of H₂O is first removed through the bottom of the stripping tower, and then the light components are removed at the top of the distillation tower. The bottom of the tower produces CO₂ products with a purity of 0.99999. A large amount of unused CO₂ at the bottom of the stripping tower and the top of the distillation tower is transported to the NaHCO₃ production process as raw materials. To reduce production energy consumption, pinch point technology is used for energy analysis, and thermal integration is achieved through dual effect distillation and heat exchange network, with a heat recovery rate of 280167.6 kJ/h. (3) The production of NaHCO₃ adopts the sodium sulfate carbonation method, and the cheap and easily available sodium mirabilite, NH₃, and CO₂ are used to react in the Oslo crystallizer to obtain NaHCO₃ crystals. The effects of NH₃, Na₂SO₄, temperature, and pressure on the crystallizer were analyzed. The results showed that the increase of NH₃ feed flow rate, it is beneficial for CO₂ capture, but excessive NH₃ will produce by-product NH₄HCO₃; The CO₂ capture rate increases with the increase of mirabilite dosage; Excessive crystallization temperature is not conducive to the capture of CO₂ and the crystallization of sodium bicarbonate; Pressure has little effect on the reaction. The final reaction conditions were determined, with a crystallization temperature of 35.5 ℃ and atmospheric pressure operation. Ammonia was used as the limiting reactant, and saturated mirabilite was fed. The feed molar ratio was Na₂SO₄: CO₂: NH₃ = 1.2:2:1. (4) Regarding the mixture of by-products Na₂SO₄ and (NH₄)₂SO₄, the strong alkali ammonia evaporation method for recovering ammonia gas was first explored, and the results showed that this method was not suitable. Based on the solubility curve, a thermal recrystallization method was developed to separate by-products. Due to the lack of relevant literature parameters, an evaporation cooling method was designed to separate by-products. The simulation process parameters were determined through experimental data, and 80.32% sodium sulfate and 22.31% ammonium sulfate were ultimately recovered from the tail liquid.

Finally, through the analysis of the whole process economy by Aspen Process Economic Analyzer V11.0, it can be seen that the project will begin to be profitable in 6.45 years, and the net rate of return will be 14.73 %, indicating that the project has certain economic benefits.

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