化学吸收法捕集二氧化碳是最具有大规模应用潜力的减碳技术。CO2的液相吸收剂经历了多代的研发，包括单一的胺溶液、混合胺溶液、离子液体、两相吸收剂和少水溶剂等，但仍不同程度地存在富液粘度较高、胺降解严重、腐蚀性高、解吸能耗高等问题。本文通过引入物理溶剂，建立化学与物理混合溶液体系，实现CO2富载溶液的液-液分相及吸收剂基础物性的改善，从而有效地降低CO2的解吸能耗。本文以MEA、DETA和BDA为主吸收剂，TMS、DGM、NPR、DMSO作为物理分相剂，对10种化学物理混合两相吸收剂进行研究，通过吸收解吸实验，定量分析了物理溶剂对分相过程的影响，获得了两相吸收剂循环吸收性能及分相过程组分迁移规律，揭示了物理溶剂促进液液分相的机理。本文研究了DGM、DMSO、TMS三种物理溶剂对两相吸收剂的密度、粘度及CO2物理溶解度的影响，分析指出化学物理类两相吸收剂粘度特性优于混合胺类两相吸收剂；DGM和TMS的添加都能改善CO2在两相吸收剂中的物理溶解度。利用填料塔装置测定了两相吸收剂的解吸能耗，结果表明化学物理两相吸收剂能够降低解吸能耗23%-59%。对MEA-TMS类两相吸收剂解吸过程的深入分析表明，TMS的添加和液液分相的发生能够显著降低解吸过程的显热和潜热，富液各组分浓度的提高对潜热的降低有一定限度。进一步的MEA-TMS-H2O-CO2体系的气液平衡研究表明，TMS的添加有利于解吸的发生，具有降低解吸能耗的作用。本文对化学物理两相吸收剂的传质特性开展了实验和模拟研究。湿壁塔实验研究表明TMS、DGM、DMSO等物理溶剂能有效提升总传质系数；分子动力学模拟研究了化学物理两相溶剂的CO2溶解性及气液界面特性，揭示了物理溶剂对气液传质过程的影响机理，提出物理溶剂能够通过改善界面捕集特性和液相组分扩散特性提高传质性能；利用动态模型研究了两相溶剂吸收CO2的传质过程，揭示了物理溶剂、氨基甲酸盐对两相吸收剂体系捕集CO2过程的影响机理。化学物理两相吸收剂具有较优的吸收性能、传质性能、粘度特性及较低的解吸能耗，具备工业应用的潜质。化学物理两相吸收剂体系的热力学模型建立是后续研究的重点，将有助于两相体系过程模拟及最优运行参数的获得。

CO2 chemical absorption is the most potential carbon reduction technology for large-scale application. CO2 aqueous absorbents have been researched and developed for many generations, including single amine solution, aqueous amine blends, as well as some research hotspot in recent years, such as ionic liquids, biphasic absorbents and less water absorbents. However, there are still some problems, such as high viscosity, serious amine degradation, high corrosiveness and high energy penalty.In this work, physical solvents were chosen as phase separation accerator added into aqueous amine solutions. The novel chemical-physical biphasic solvents were demonstrated to have better capacity and the phase splitting phenomenon is potential to reduce energy penalty.Ten kinds of chemical-physical biphasic solvents were screened out by absorption and desorption experiments. It is suggested that MEA, DETA and BDA are excellent main absorbents, and TMS, DGM, NPR and DMSO are suitable physical phase separation accelerators. The phase separation process was quantitatively analyzed and the mechanism of physical solvents promoting phase separation was revealed. The effects of DGM, DMSO and TMS on the density, viscosity and physical solubility of chemical-physical biphasic solvents were studied. It is pointed out that the viscosity of chemical-physical biphasic solvents is lower than that of mixed amine biphasic solvents. And the addition of DGM and TMS can improve the physical solubility of CO2 in biphasic solvents.The desorption energy consumption of chemical-physical biphasic solvents was measured by using the packed tower apparatus. The results show that the biphasic solvents can reduce the desorption energy consumption by 23% - 59%. The desorption process of MEA-TMS biphasic solvent was analyzed. The results show that the addition of TMS and the occurrence of liquid-liquid phase splitting can significantly reduce the sensible heat and latent heat of the desorption process, and the increase of the concentration of each component has a certain limit on the reduction of latent heat. Further study on the gas-liquid equilibrium of MEA-TMS-H2O-CO2 system shows that the addition of TMS is beneficial to CO2 desorption and can reduce the desorption energy consumption.In this paper, the mass transfer characteristics of chemical-physical biphasic solvents were studied by the wetted-wall column experiments and molecular dynamic simulation. The experimental results show that TMS, DGM, DMSO can effectively improve the total mass transfer coefficient. Molecular dynamics simulation were used to study the CO2 solubility and gas-liquid interface characteristics of chemical-physical biphasic solvents. The study revealed the mechanism of gas-liquid mass transfer process of biphasic solvents, and proposed that the physical solvents can improve the mass transfer performance by promoting the interface CO2 capture characteristics and CO2 diffusion coefficient in liquid phase. Then the mass transfer process of CO2 absorption by biphasic solvents was studied by using a new dynamic model, the influence of physical solvents and carbamate on CO2 capture process of biphasic solvents were studied.Chemical-physical biphasic solvents have better absorption performance, mass transfer performance, viscosity characteristics and lower desorption energy consumption, which has the potential of industrial application. The establishment of thermodynamic model of chemical-physical biphasic system is the focus of follow-up research, which will be helpful to the process simulation and the determination of optimal operation parameters.