Effect of acids produced by the dissolution of sulfur and nitrogen oxides in the performance of MEA solvent in CO2 capture: Experimental results and modeling

IF 2.7 3区 工程技术 Q3 CHEMISTRY, PHYSICAL Fluid Phase Equilibria Pub Date : 2025-04-01 Epub Date: 2024-12-04 DOI:10.1016/j.fluid.2024.114309
Fragkiskos Tzirakis , Ioannis Tsivintzelis , Panos Seferlis , Athanasios I. Papadopoulos
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Abstract

Solvent-based CO2 capture is very important for the mitigation of greenhouse gases. The presence of SO2 and NO2 is observed in several types of CO2-containing industrial flue gases and even small concentrations can cause significant changes in the performance of the solvent. Their effects on the CO2 solubility have received very little attention. To simulate the effect of dissolution and accumulation of SO2 and NO2 acid gases on the CO2 loading of aqueous ethanolamine (MEA) solutions, H2SO4 and HNO3 were added, as sources of NO3 and SO42 anions, respectively. The CO2 solubility in 30 % wt. aqueous MEA solutions containing 2.9 % wt. H2SO4 with and without 1.8 % wt. HNO3 was experimentally measured using a pressure decay method at 313, 333 and 353 K and approximately 5–500 kPa. In both cases, it is revealed that the addition of H2SO4 and HNO3 substantially decreases the CO2 solubility. In addition, the modified Kent-Eisenberg model was used to predict the CO2 solubility in all systems and at all the studied conditions. The model predictions are in satisfactory agreement with the experimental data presenting Average Absolute Deviations between 4.8 and 6.8 % in all cases.

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硫和氮氧化物溶解产生的酸对MEA溶剂CO2捕集性能的影响:实验结果和建模
溶剂型CO2捕集对于减缓温室气体非常重要。在几种含二氧化碳的工业烟气中观察到SO2和NO2的存在,即使浓度很小也会导致溶剂性能的显著变化。它们对CO2溶解度的影响很少受到关注。为了模拟SO2和NO2酸性气体的溶解和积累对乙醇胺水溶液中CO2负荷的影响,分别加入H2SO4和HNO3作为NO3−和SO4−2阴离子的来源。采用压力衰减法,在313、333和353 K,约5-500 kPa的条件下,实验测量了CO2在含有2.9% wt. H2SO4和不含1.8% wt. HNO3的30% wt. MEA水溶液中的溶解度。在这两种情况下,H2SO4和HNO3的加入都显著降低了CO2的溶解度。此外,采用改进的Kent-Eisenberg模型预测了CO2在所有体系和所有研究条件下的溶解度。模型预测结果与实验数据吻合较好,平均绝对偏差在4.8 ~ 6.8%之间。
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来源期刊
Fluid Phase Equilibria
Fluid Phase Equilibria 工程技术-工程:化工
CiteScore
5.30
自引率
15.40%
发文量
223
审稿时长
53 days
期刊介绍: Fluid Phase Equilibria publishes high-quality papers dealing with experimental, theoretical, and applied research related to equilibrium and transport properties of fluids, solids, and interfaces. Subjects of interest include physical/phase and chemical equilibria; equilibrium and nonequilibrium thermophysical properties; fundamental thermodynamic relations; and stability. The systems central to the journal include pure substances and mixtures of organic and inorganic materials, including polymers, biochemicals, and surfactants with sufficient characterization of composition and purity for the results to be reproduced. Alloys are of interest only when thermodynamic studies are included, purely material studies will not be considered. In all cases, authors are expected to provide physical or chemical interpretations of the results. Experimental research can include measurements under all conditions of temperature, pressure, and composition, including critical and supercritical. Measurements are to be associated with systems and conditions of fundamental or applied interest, and may not be only a collection of routine data, such as physical property or solubility measurements at limited pressures and temperatures close to ambient, or surfactant studies focussed strictly on micellisation or micelle structure. Papers reporting common data must be accompanied by new physical insights and/or contemporary or new theory or techniques.
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