T = 25℃时HF- naf - h2o和HF- kf - h2o混合体系高达2 m HF固液平衡模型

Stanislav Donchev, Tsvetan Tsenov, C. Christov
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摘要

摘要在本研究中,我们开发了HF-NaF-H2O和HF-KF-H2O混合系统在T=25℃下高达2 m HF的固液平衡热力学模型。模型是在Pitzer离子相互作用方法的基础上开发的。利用平均活度系数(γ±)的建议建立了HF-H2O系统的模型。NaF-H2O和KF-H2O二元系统的模型取自我们之前在同一期刊上的研究[Donchev等人ASN(2021)8(2),1-15]。为了参数化三元体系的模型,我们使用了可用的溶解度数据,即基于溶解度方法。基于评估的模型离子相互作用参数和使用实验m(sat)溶解度数据,确定了在混合体系中沉淀的热力学溶解度产物(如ln-Kosp)复盐[NaF.HF(cr)和KF.HF(cr)]。该模型与HF–NaF–H2O和HF–NaF–H2O体系中的经验溶解度数据非常一致,最大HF摩尔浓度为2 mol·kg−1。在较高的酸摩尔浓度下,该模型预测两种混合体系的复盐(NaF.HF(cr)和KF.HF(cr))的溶解度要高得多。得出的结论是,参数化中使用的二元HF–H2O系统的原始数据不正确是本文提出的混合HF模型的浓度限制的主要原因。
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Thermodynamic solid-liquid equilibrium model for mixed systems HF-NaF-H2O and HF-KF-H2O up to 2 m HF at T = 25oC
Abstract In this study we developed thermodynamic models for solid-liquid equilibrium for mixed systems HF-NaF-H2O and HF-KF-H2O up to 2 m HF at T = 25oC. Models are developed on the basis of Pitzer ion interactions approach. The recommendations on mean activity coefficients (γ±) have been used to construct the model for HF-H2O system. The models for binary systems NaF-H2O and KF-H2O are taken from our previous study in the same journal [Donchev et al. ASN (2021) 8(2), 1-15]. To parameterize models for ternary systems we used the available solubility data, i.e. on the basis of solubility approach. The thermodynamic solubility products (as ln Kosp) of precipitating in mixed systems double salts [NaF.HF(cr), and KF.HF(cr)] have been determined on the basis of evaluated model ion interaction parameters and using experimental m(sat) solubility data. The model is in a good agreement with experimewnt solubility data in the systems HF–NaF–H2O and HF–NaF–H2O up to maximum HF molality of 2 mol·kg−1. At higher acid molality the model predicts much higher solubility of double salts (NaF.HF(cr) and KF.HF(cr) for both mixed systems. It was concluded that not a correct raw data for binary HF–H2O system used in parameterization are the main reason for concentration restriction of mixed HF models presented here.
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