N2在液相/密相CO2中溶解过程的试验及分子动力学研究

N2 in liquid phase/dense phase CO2 dissolved in the process of test and the molecular dynamics research

  • 摘要: 煤炭开采与使用中的碳排放是导致全球变暖的原因之一,为减少CO2排放、实现“双碳”目标,必须推进二氧化碳捕集、利用与封存技术(CCUS技术)的发展。CO2性质的研究是CCUS技术的基础性支撑,其中密相CO2在二氧化碳的捕集与封存阶段中均有涉及,而目前关于密相CO2性质的研究仍存在空白。因此,为进一步探究密相CO2的溶解能力,在实验室中进行了N2在液相、密相CO2中的溶解试验,获得了N2‒CO2二元混合体系在287.15 K、5~9 MPa条件下,N2在CO2中的溶解度随压强的变化规律,并通过分子动力学模拟的方法从微观角度深入分析了N2在CO2中溶解的过程。研究结果表明:在287.15 K、5~9 MPa条件下,各单一相态下N2在CO2中的溶解度与压强呈正相关,一般液态CO2中N2体积分数在14%上下波动,密相CO2中N2含量在20%上下波动,由一般液态过渡至密相使N2体积分数从13.38%突增至18.45%。分子动力学模拟的结果进一步表明:CO2分子的扩散系数、径向分布函数以及CO2分子与N2分子间的相互作用能的变化是导致密相CO2表现出更强溶解能力的直接原因,CO2分子键角以及配位数的变化仅受体系内压强变化的影响,并未直接受到CO2相态变化的影响,是导致密相CO2表现出更强溶解能力的间接原因,而CO2分子的键长并不会随体系内压强和CO2相态的变化发生明显的改变,因此不是导致密相CO2表现出更强溶解能力的原因。

     

    Abstract: Carbon emissions from coal mining and use are one of the causes of global warming, to reduce CO2 emissions and achieve the dual carbon goal, it is necessary to promote the development of carbon capture, utilization, and storage (CCUS) technology. The research on the properties of CO2 is fundamental to CCUS technology, and dense phase CO2 is involved in both the capture and storage stages of carbon dioxide. However, there is still a gap in the current research on the properties of dense phase CO2. Therefore, to further explore the dissolving ability of dense phase CO2, N2 is carried out in laboratory to dissolve in the liquid phase, dense phase CO2 test, obtained the N2. The research results show that the solubility of N2 in CO2 is positively correlated with pressure in various single phase states between 5 and 9 MPa at 287.15 K. Generally, the N2 content in liquid CO2 fluctuates around 14%, while in dense CO2 it fluctuates around 20%. The transition from general liquid to dense phase results in a sudden increase in N2 content from 13.38% to 18.45%, and the results of molecular dynamics simulation indicate that the diffusion coefficient, radial distribution function, and interaction energy between CO2 molecules and N2 molecules are the direct reasons for the stronger solubility of dense phase CO2. The changes in bond angle and coordination number of CO2 molecules are only affected by the pressure changes in the receptor system, and are not directly affected by the CO2 phase change, which is an indirect reason for the stronger solubility of dense phase CO2. The bond length of CO2 molecules does not change significantly with the pressure and CO2 phase change in the system, so it is not the reason for the stronger solubility of dense phase CO2.

     

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