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溶解于二氧化碳中的不可凝气体的亨利定律常数及气液分配系数

Henry's Law Constants and Vapor-Liquid Distribution Coefficients of Noncondensable Gases Dissolved in Carbon Dioxide.

作者信息

Martynov Sergey B, Porter Richard T J, Mahgerefteh Haroun

机构信息

Department of Chemical Engineering, University College London, Torrington Place, London WC1E 7JE, U.K.

出版信息

ACS Omega. 2022 Mar 2;7(10):8777-8788. doi: 10.1021/acsomega.1c07044. eCollection 2022 Mar 15.

Abstract

The accurate determination of the solubilities of the typical impurity gases present in captured CO in the carbon capture, utilization, and storage chain is an essential prerequisite for the successful modeling of the CO stream thermodynamic properties. In this paper, Henry's law constants and the vapor-liquid distribution coefficients of six noncondensable gases, namely, N, O, H, CH, Ar, and CO, at infinite dilution in liquid CO are derived based on published vapor-liquid equilibrium data at temperatures ranging from the triple point (216.59 K) to the critical point (304.13 K) of CO. The temperature dependence of Henry's law constants of the six gases is correlated using approximating functions previously proposed for aqueous solutions. A correlation that provides the best fit for the Henry constants data for all the six gases, with the accuracy (absolute average deviation %) of 4.2%, is recommended. For N, O, H, Ar, and CO, the combined standard uncertainty in the derived Henry constants is less than 6%, whereas for CH, due to a larger deviation between the utilized data, the uncertainty is less than 18%. Analysis of the temperature variation of the vapor-liquid distribution coefficient at infinite dilution shows that when all the six gases are present in the CO stream, separation of N, O, Ar, and CO from CO can be problematic due to their similar volatilities, while the distinct volatilities of H and CH at lower temperatures make their separation from CO easier.

摘要

准确测定碳捕集、利用与封存链中捕获的一氧化碳中典型杂质气体的溶解度,是成功模拟一氧化碳物流热力学性质的必要前提。本文基于已发表的在一氧化碳从三相点(216.59 K)到临界点(304.13 K)温度范围内的气液平衡数据,推导了六种不可凝气体,即氮气、氧气、氢气、甲烷、氩气和一氧化碳在液态一氧化碳中无限稀释时的亨利定律常数和气液分配系数。使用先前针对水溶液提出的近似函数来关联这六种气体亨利定律常数的温度依赖性。推荐了一种能对所有六种气体的亨利常数数据提供最佳拟合的关联式,其准确度(绝对平均偏差%)为4.2%。对于氮气、氧气、氢气、氩气和一氧化碳,推导得到的亨利常数的合成标准不确定度小于6%,而对于甲烷,由于所用数据之间偏差较大,不确定度小于18%。对无限稀释时气液分配系数的温度变化分析表明,当一氧化碳物流中存在所有六种气体时,由于氮气、氧气、氩气和一氧化碳挥发性相似,将它们与一氧化碳分离可能存在问题,而氢气和甲烷在较低温度下挥发性不同,使得它们与一氧化碳的分离更容易。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e8c9/8928534/cafa201c9ce2/ao1c07044_0002.jpg

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