FAN Yongsheng, GONG Haiting, LI Cai, et al. Carbon capture performance and mechanism of MCA/EG steric hindrance non-aqueous absorbent[J]. Thermal power generation, 2025, 54(6): 105-112.
FAN Yongsheng, GONG Haiting, LI Cai, et al. Carbon capture performance and mechanism of MCA/EG steric hindrance non-aqueous absorbent[J]. Thermal power generation, 2025, 54(6): 105-112. DOI: 10.19666/j.rlfd.202412271.
MCA/EG空间位阻非水体系碳捕集性能及机理研究
摘要
碳捕集、利用与封存技术是我国实现“双碳”目标的重要途径,其中非水吸收剂具有巨大的节能潜力,且适配现有吸收法混胺反应器,具有较大应用潜力,但存在CO_2饱和溶液黏度大、循环负荷低等问题。对此,以仲胺MCA为吸收组分,EG为有机溶剂,构建了低黏度、低温再生非水吸收体系,并考察了MCA/EG的吸收、再生性能。结果表明:3mol/L MCA/EG吸收剂的吸收负荷可达2.14 mol/L,黏度仅为44.19 m Pa·s;在40℃吸收30 min、80℃再生25 min条件下,循环负荷高达0.98 mol/L,为质量分数为30%的MEA/H_2O溶液在105.5℃再生条件下循环负荷的1.46倍。通过C80微量热仪测试得到吸收剂的反应热为–82.85 k J/mol,低于MEA/H_2O溶液。结合~(13)C NMR与量子化学计算,探究了吸收剂捕集CO_2的反应机理,发现MCA的空间位阻效应降低了反应产物的稳定性,使氨基甲酸酯与EG进一步反应转化为烷基碳酸酯,降低了再生难度,实现了低温再生。该吸收体系可实现非水吸收剂的稳定运行,并扩大吸收剂再生中的余热利用范围,具有较大的降能耗优势。
Abstract
Carbon capture
utilization and storage technology is an important way to realize the carbon peaking and carbon neutrality goals in China. Among them
the non-aqueous phase absorbents have great energy-saving potential
and it is suitable for the existing mixed amine reactor
which has a large development potential.However
there are still problems such as high viscosity of CO_2 saturated solution and low circulating load. In this regard
a non-aqueous absorption system with low viscosity and regeneration temperature was constructed using secondary amine MCA as the absorbing component and EG as the organic solvent. The absorption and regeneration performance of MCA/EG was investigated. The results showed that
the absorption load of 3 mol/L MCA/EG solvent was up to 2.14 mol/L
and the viscosity was only 44.19 m Pa·s. Under the condition of absorption at 40 ℃ for 30 min and regeneration at 80 ℃ for 25 min
the cyclic load was as high as 0.98 mol/L
which is 1.46 times of the cyclic load of 30% MEA/H_2O solution at 105.5 ℃. The reaction heat of the absorbent was measured to be-82.85 kJ/mol by C80 microcalorimeter
which was lower than that of the MEA/H2O solution. The reaction mechanism of CO_2 capture by MCA/EG was explored by ~(13)C NMR and quantum chemical calculations. It was found that the stability of the reaction products was reduced for the steric hindrance effect of MCA. The carbamates transform into alkyl carbonate by reacting with EG to realize the regeneration at low temperatures. MCA/EG can realize the stable operation of non-aqueous phase absorbent and expand the scope of waste heat utilization in absorbent regeneration