Dissolution and Solubility of the Synthetic Natroalunite and the Arsenic-Incorporated Natroalunite at pH of 2.00–5.60 and 25–45°C

Arsenic is very harmful to most living organisms. The solubility data of As-containing compounds are significant in geoscience and environmental science. The arsenic-incorporated natroalunite precipitation has been proposed to eliminate arsenic from water, both for industrial practice and remediatio...

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Main Authors: Yinian Zhu, Huiling Xuan, Yanpeng Liang, Qiming Yan, Zongqiang Zhu, Zhangnan Jiang, Lihao Zhang, Huili Liu, Shen Tang
Format: Article
Language:English
Published: Wiley 2019-01-01
Series:Journal of Chemistry
Online Access:http://dx.doi.org/10.1155/2019/9568360
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author Yinian Zhu
Huiling Xuan
Yanpeng Liang
Qiming Yan
Zongqiang Zhu
Zhangnan Jiang
Lihao Zhang
Huili Liu
Shen Tang
author_facet Yinian Zhu
Huiling Xuan
Yanpeng Liang
Qiming Yan
Zongqiang Zhu
Zhangnan Jiang
Lihao Zhang
Huili Liu
Shen Tang
author_sort Yinian Zhu
collection DOAJ
description Arsenic is very harmful to most living organisms. The solubility data of As-containing compounds are significant in geoscience and environmental science. The arsenic-incorporated natroalunite precipitation has been proposed to eliminate arsenic from water, both for industrial practice and remediation of polluted areas. Unfortunately, only few works have been made on partial arsenic incorporation in natroalunite and the thermodynamic data for natroalunite and arsenic-incorporated natroalunite now are still lacking. Moreover, the dissolution mechanisms of arsenic-incorporated natroalunites have never been studied. In the present work, the dissolution of the synthetic natroalunite [Na0.93(H3O)0.61Al2.82(SO4)2(OH)6] and the synthetic arsenic-incorporated natroalunite [Na0.88(H3O)2.44Al2.35(AsO4)0.38(SO4)1.62(OH)6] at 25°C, 35°C, and 45°C was experimentally examined in HNO3 solution (pH of 2.00 and 4.00) and pure water. The characterizations confirmed that the solids showed no recognizable change after dissolution. All dissolutions underwent a pH variation, which was caused by a great depleting of H3O+/OH− ions, typically at the reaction beginning. The dissolution in H3O+ medium proved to be near-stoichiometric within the short beginning period, and the dissolved Na+, Al3+, SO42−, and AsO43− concentrations were stoichiometric according to the initial solids and then appeared to be nonstoichiometric with the Na/SO4 mole ratios higher and the Al/SO4 and AsO4/SO4 mole ratios lower than the stoichiometry until the experimental end, indicating that the components were released from solid to solution preferentially after the following order: Na+ (H3O+) > SO42− > AsO43− > Al3+. From the experimental results under the condition of initial pH 2.00 and 25°C, the solubility products [Ksp] and the Gibbs free energies of formation [ΔGf°] were calculated to be 10−81.02±0.33∼10−81.04±0.27 and −4713 ± 2 to −4714 ± 1 kJ/mol for the natroalunite and 10−92.30±0.30∼10−92.41±0.37 and −5078 ± 2 to −5079 ± 2 kJ/mol for the arsenic-incorporated natroalunite, respectively. The thermodynamic quantities, ΔG°, ΔH°, ΔS°, and ΔCp°, were determined to be 462303.43 J/K·mol, 122466.83 J/mol, −1140.39 J/K·mol, and 4280.13 J/K·mol for the natroalunite dissolution reaction at initial pH 2.00 and 25°C and to be 526925.48 J/K·mol, 159674.76 J/mol, −1232.38 J/K·mol, and 1061.12 J/K·mol for the dissolution of the arsenic-incorporated natroalunite at initial pH 2.00 and 25°C, respectively.
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spelling doaj-art-932519fafc604becbc8d233d9981430e2025-02-03T05:58:07ZengWileyJournal of Chemistry2090-90632090-90712019-01-01201910.1155/2019/95683609568360Dissolution and Solubility of the Synthetic Natroalunite and the Arsenic-Incorporated Natroalunite at pH of 2.00–5.60 and 25–45°CYinian Zhu0Huiling Xuan1Yanpeng Liang2Qiming Yan3Zongqiang Zhu4Zhangnan Jiang5Lihao Zhang6Huili Liu7Shen Tang8College of Environmental Science and Engineering, Guilin University of Technology, Guilin 541004, ChinaCollege of Environmental Science and Engineering, Guilin University of Technology, Guilin 541004, ChinaGuangxi Key Laboratory of Environmental Pollution Control Theory and Technology, Guilin University of Technology, Guilin 541004, ChinaCollege of Environmental Science and Engineering, Guilin University of Technology, Guilin 541004, ChinaCollege of Environmental Science and Engineering, Guilin University of Technology, Guilin 541004, ChinaCollege of Environmental Science and Engineering, Guilin University of Technology, Guilin 541004, ChinaGuangxi Key Laboratory of Environmental Pollution Control Theory and Technology, Guilin University of Technology, Guilin 541004, ChinaCollege of Environmental Science and Engineering, Guilin University of Technology, Guilin 541004, ChinaGuangxi Key Laboratory of Environmental Pollution Control Theory and Technology, Guilin University of Technology, Guilin 541004, ChinaArsenic is very harmful to most living organisms. The solubility data of As-containing compounds are significant in geoscience and environmental science. The arsenic-incorporated natroalunite precipitation has been proposed to eliminate arsenic from water, both for industrial practice and remediation of polluted areas. Unfortunately, only few works have been made on partial arsenic incorporation in natroalunite and the thermodynamic data for natroalunite and arsenic-incorporated natroalunite now are still lacking. Moreover, the dissolution mechanisms of arsenic-incorporated natroalunites have never been studied. In the present work, the dissolution of the synthetic natroalunite [Na0.93(H3O)0.61Al2.82(SO4)2(OH)6] and the synthetic arsenic-incorporated natroalunite [Na0.88(H3O)2.44Al2.35(AsO4)0.38(SO4)1.62(OH)6] at 25°C, 35°C, and 45°C was experimentally examined in HNO3 solution (pH of 2.00 and 4.00) and pure water. The characterizations confirmed that the solids showed no recognizable change after dissolution. All dissolutions underwent a pH variation, which was caused by a great depleting of H3O+/OH− ions, typically at the reaction beginning. The dissolution in H3O+ medium proved to be near-stoichiometric within the short beginning period, and the dissolved Na+, Al3+, SO42−, and AsO43− concentrations were stoichiometric according to the initial solids and then appeared to be nonstoichiometric with the Na/SO4 mole ratios higher and the Al/SO4 and AsO4/SO4 mole ratios lower than the stoichiometry until the experimental end, indicating that the components were released from solid to solution preferentially after the following order: Na+ (H3O+) > SO42− > AsO43− > Al3+. From the experimental results under the condition of initial pH 2.00 and 25°C, the solubility products [Ksp] and the Gibbs free energies of formation [ΔGf°] were calculated to be 10−81.02±0.33∼10−81.04±0.27 and −4713 ± 2 to −4714 ± 1 kJ/mol for the natroalunite and 10−92.30±0.30∼10−92.41±0.37 and −5078 ± 2 to −5079 ± 2 kJ/mol for the arsenic-incorporated natroalunite, respectively. The thermodynamic quantities, ΔG°, ΔH°, ΔS°, and ΔCp°, were determined to be 462303.43 J/K·mol, 122466.83 J/mol, −1140.39 J/K·mol, and 4280.13 J/K·mol for the natroalunite dissolution reaction at initial pH 2.00 and 25°C and to be 526925.48 J/K·mol, 159674.76 J/mol, −1232.38 J/K·mol, and 1061.12 J/K·mol for the dissolution of the arsenic-incorporated natroalunite at initial pH 2.00 and 25°C, respectively.http://dx.doi.org/10.1155/2019/9568360
spellingShingle Yinian Zhu
Huiling Xuan
Yanpeng Liang
Qiming Yan
Zongqiang Zhu
Zhangnan Jiang
Lihao Zhang
Huili Liu
Shen Tang
Dissolution and Solubility of the Synthetic Natroalunite and the Arsenic-Incorporated Natroalunite at pH of 2.00–5.60 and 25–45°C
Journal of Chemistry
title Dissolution and Solubility of the Synthetic Natroalunite and the Arsenic-Incorporated Natroalunite at pH of 2.00–5.60 and 25–45°C
title_full Dissolution and Solubility of the Synthetic Natroalunite and the Arsenic-Incorporated Natroalunite at pH of 2.00–5.60 and 25–45°C
title_fullStr Dissolution and Solubility of the Synthetic Natroalunite and the Arsenic-Incorporated Natroalunite at pH of 2.00–5.60 and 25–45°C
title_full_unstemmed Dissolution and Solubility of the Synthetic Natroalunite and the Arsenic-Incorporated Natroalunite at pH of 2.00–5.60 and 25–45°C
title_short Dissolution and Solubility of the Synthetic Natroalunite and the Arsenic-Incorporated Natroalunite at pH of 2.00–5.60 and 25–45°C
title_sort dissolution and solubility of the synthetic natroalunite and the arsenic incorporated natroalunite at ph of 2 00 5 60 and 25 45°c
url http://dx.doi.org/10.1155/2019/9568360
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