In this work, a molecular simulation method was used to study the adsorption of seven combustion products (CO₂, H₂O, SO₂, N₂, O₂, NO and NO₂) on three zeolites with different topological structures (4A, MIF and MOR). Adsorption isotherms of pure components and mixtures at a wide range of temperatures (253–333 K) were calculated using the Monte Carlo method, obtaining equilibrium parameters including the adsorption capacity, adsorption heat and energy distribution. The calculation results indicated that 4A zeolite with more micropores has a stronger adsorption performance for CO₂. The presence of water significantly reduced the CO₂ capture efficiency of the three zeolites, and the CO₂ adsorption amount decreased by more than 80%. Adsorption kinetics was studied using the molecular dynamic (MD) method, MFI and MOR, with channel-type pore structures exhibiting stronger gas diffusion performance, though their separation efficiency was not high. A 4A zeolite has the potential for kinetic separation of CO₂.

While nuclear energy represents a low‐carbon and high‐efficiency energy source that plays a vital role in the global energy mix, the limitations of spent fuel reprocessing technology pose a major challenge to its sustainable development. The PUREX (plutonium uranium redox extraction) process is currently the dominant nuclear fuel reprocessing technology in the world. However, the key extractant in this process is tributyl phosphate (TBP), which degrades under intense radiation, high temperatures, and strong acidity. This leads to the production of dibutyl phosphate, monobutyl phosphate, and other degradation byproducts, which may reduce the extraction efficiency and trigger third‐phase formation and equipment corrosion. This paper systematically reviews the degradation mechanisms of TBP and its diluents, the analytical technique suitable for characterizing degradation products, and the impact of degradation products on the post‐treatment process. Additionally, optimization strategies employed for suppressing third‐phase formation are discussed. This study offers a theoretical foundation and technical insights in optimizing the PUREX process and ensuring the safe operation of the post‐treatment process.