Thermodynamic and chemical properties of liquid carbon dioxide and nitrogen（CO_（2~–）N_2） mixture under the conditions of extremely high densities and temperatures are studied by using quantum molecular dynamic（...Thermodynamic and chemical properties of liquid carbon dioxide and nitrogen（CO_（2~–）N_2） mixture under the conditions of extremely high densities and temperatures are studied by using quantum molecular dynamic（QMD） simulations based on density functional theory including dispersion corrections（DFT-D）. We present equilibrium properties of liquid mixture for 112 separate density and temperature points, by selecting densities ranging from ρ = 1.80 g/cm^3 to 3.40 g/cm^3 and temperatures from T = 500 K to 8000 K. In the range of our study, the liquid CO_（2~–）N_2 mixture undergoes a continuous transition from molecular to atomic fluid state and liquid polymerization inferred from pair correlation functions（PCFs）and the distribution of various molecular components. The insulator–metal transition is demonstrated by means of the electronic density of states（DOS）.展开更多
The high price and toxicity of ionic liquids(ILs) have limited the design and application of supported ionic liquid membranes(SILMs) for CO_2 separation in both academic and industrial fields. In this work, [Choline][...The high price and toxicity of ionic liquids(ILs) have limited the design and application of supported ionic liquid membranes(SILMs) for CO_2 separation in both academic and industrial fields. In this work, [Choline][Pro]/polyethylene glycol 200(PEG200) mixtures were selected to prepare novel SILMs because of their green and costeffective characterization, and the CO_2/N_2 separation with the prepared SILMs was investigated experimentally at temperatures from 308.15 to 343.15 K. The temperature effect on the permeability, solubility and diffusivity of CO_2 was modeled with the Arrhenius equation. A competitive performance of the prepared SILMs was observed with high CO_2 permeability ranged in 343.3–1798.6 barrer and high CO_2/N_2 selectivity from 7.9 to 34.8.It was also found that the CO_2 permeability increased 3 times by decreasing the viscosity of liquids from 370 to38 m Pa·s. In addition, the inherent mechanism behind the significant permeability enhancement was revealed based on the diffusion-reaction theory, i.e. with the addition of PEG200, the overall resistance was substantially decreased and the SILMs process was switched from diffusion-control to reaction-control.展开更多
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11374217,11135012,and 11375262)the Joint Fund of the National Natural Science Foundation of Chinathe China Academy of Engineering Physics(Grant No.11176020)
文摘Thermodynamic and chemical properties of liquid carbon dioxide and nitrogen（CO_（2~–）N_2） mixture under the conditions of extremely high densities and temperatures are studied by using quantum molecular dynamic（QMD） simulations based on density functional theory including dispersion corrections（DFT-D）. We present equilibrium properties of liquid mixture for 112 separate density and temperature points, by selecting densities ranging from ρ = 1.80 g/cm^3 to 3.40 g/cm^3 and temperatures from T = 500 K to 8000 K. In the range of our study, the liquid CO_（2~–）N_2 mixture undergoes a continuous transition from molecular to atomic fluid state and liquid polymerization inferred from pair correlation functions（PCFs）and the distribution of various molecular components. The insulator–metal transition is demonstrated by means of the electronic density of states（DOS）.
基金Supported by the National Basic Research Program of China(2013CB733501)the National Natural Science Foundation of China(21136004,21176112,21476106,and21428601)+1 种基金Specialized Research Fund for the Doctoral Program of Higher Education(No.20133221110001)the Project of Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)
文摘The high price and toxicity of ionic liquids(ILs) have limited the design and application of supported ionic liquid membranes(SILMs) for CO_2 separation in both academic and industrial fields. In this work, [Choline][Pro]/polyethylene glycol 200(PEG200) mixtures were selected to prepare novel SILMs because of their green and costeffective characterization, and the CO_2/N_2 separation with the prepared SILMs was investigated experimentally at temperatures from 308.15 to 343.15 K. The temperature effect on the permeability, solubility and diffusivity of CO_2 was modeled with the Arrhenius equation. A competitive performance of the prepared SILMs was observed with high CO_2 permeability ranged in 343.3–1798.6 barrer and high CO_2/N_2 selectivity from 7.9 to 34.8.It was also found that the CO_2 permeability increased 3 times by decreasing the viscosity of liquids from 370 to38 m Pa·s. In addition, the inherent mechanism behind the significant permeability enhancement was revealed based on the diffusion-reaction theory, i.e. with the addition of PEG200, the overall resistance was substantially decreased and the SILMs process was switched from diffusion-control to reaction-control.
