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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Thermodynamic Dissociation Constant of the Bisulfate Ion from Raman and Ion Interaction Modeling Studies of Aqueous Sulfuric Acid at Low Temperatures
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Thermodynamic Dissociation Constant of the Bisulfate Ion from Raman and Ion Interaction Modeling Studies of Aqueous Sulfuric Acid at Low Temperatures

机译：拉曼硫酸氢根离子的热力学解离常数和硫酸水溶液在低温下的离子相互作用模型研究

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摘要

The dissociation reaction of the bisulfate ion, HSO_4~- ＜＝＞ SO_4~(2-) + H~+, is investigated in aqueous H_2SO_4 solutions with concentrations of 0.54-15.23 mol kg~(-1) in the temperature range of 180-326 K using Raman spectroscopy. All investigated H_2SO_4 solutions show a continuous increase in the degree of dissociation of HSO_4~- with decreasing temperature, in contrast to predictions from thermodynamic models of aqueous H_2SO_4 solutions. A Pitzer ion interaction model is used to derive a thermodynamically consistent formulation of the thermodynamic dissociation constant of the bisulfate ion, K_(II)(T), that is in agreement with the experimental data. The new formulation of K_(II)(T) is valid from 180 to 473 K. All ion interaction parameters and the corresponding parametrizations of the Pitzer ion interaction model are presented. Calculations with this model reveal significant differences in ion activity coefficients, water activities, water vapor pressure, and HCl solubilities, when compared to existing thermodynamic models of H_2SO_4/H_2O solutions, in particular at lower temperatures.
机译：研究了硫酸氢根离子HSO_4〜-＜＝＞ SO_4〜（2-）+ H〜+的离解反应，其温度为180℃，浓度为0.54-15.23 mol kg〜（-1）的H_2SO_4水溶液。使用拉曼光谱法测定-326K。与根据H_2SO_4水溶液的热力学模型所作的预测相反，所有研究的H_2SO_4溶液均显示HSO_4〜-的解离度随着温度的降低而持续增加。使用皮茨离子相互作用模型来得出硫酸氢根离子K_（II）（T）的热力学解离常数的热力学一致性公式，与实验数据相符。 K_（II）（T）的新公式在180到473 K之间有效。介绍了所有离子相互作用参数以及Pitzer离子相互作用模型的相应参数。与现有的H_2SO_4 / H_2O溶液的热力学模型相比，尤其是在较低温度下，使用该模型进行的计算显示出离子活度系数，水活度，水蒸气压力和HCl溶解度存在显着差异。

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