{"title":"以 Fe(OH)3 为固体铁源在含砷溶液中形成蝎尾石的机制和动力学","authors":"","doi":"10.1016/j.psep.2024.09.055","DOIUrl":null,"url":null,"abstract":"<div><p>Recently, solid iron sources have been used for scorodite synthesis in arsenic-bearing wastewater from nonferrous metallurgy. Immobilising arsenic-solution as scorodite via iron hydroxide (Fe(OH)<sub>3</sub>) solid iron source is an important method for controlling arsenic pollution. The evolution behavior of scorodite during its formation in high arsenic solution have been rarely investigated. In this paper, the mechanism and kinetics of scorodite formation using Fe(OH)<sub>3</sub> in arsenic-bearing solution were investigated. This work was divided into three parts. Firstly, the influencing parameters were investigated, revealing that the dissolution of Fe(OH)<sub>3</sub> and scorodite generation accelerated at lower initial pH and higher reaction temperature. Increasing Fe/As ratio delayed scorodite crystallisation, which was in turn enhanced by elevating arsenic concentration. Secondly, the mechanism of scorodite formation was investigated, revealing that Fe(OH)<sub>3</sub> underwent acidic dissolution to form a precursor. Subsequent scorodite formation had a Δ<sub>r</sub>G<sub>m</sub><sup>θ</sup> ranging from −69.39 kJ·mol<sup>−1</sup> to −15.64 kJ·mol<sup>−1</sup>. Residual As was absorbed and converted into Fe(OH)<sub>3</sub>@scorodite. Thirdly, the chemical kinetics were investigated, showing that activation energy (Ea) for Fe(OH)<sub>3</sub> dissolution was 72.54 and 105.37 kJ·mol<sup>−1</sup> at Stages I and II, respectively, whereas it was 105.97 kJ·mol<sup>−1</sup> for residual As absorption-conversion at Stage III outweighing the Ea of As-Fe coprecipitation. The restrictive steps were Fe(OH)<sub>3</sub> dissolution and residual arsenic absorption-conversion. This proposed method can be applied for environment-friendly treatment of 10-40 g/L of arsenic-bearing industrial effluent for scorodite formation. Overall, this research confirmed the formation of scorodite via Fe(OH)<sub>3</sub> and can potentially provide feasible schemes for eliminating arsenic-bearing acidic waste, dust, and anode slime from nonferrous metallurgical processes.</p></div>","PeriodicalId":20743,"journal":{"name":"Process Safety and Environmental Protection","volume":null,"pages":null},"PeriodicalIF":6.9000,"publicationDate":"2024-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Mechanism and kinetics of scorodite formation in arsenic-bearing solutions using Fe(OH)3 as a solid iron source\",\"authors\":\"\",\"doi\":\"10.1016/j.psep.2024.09.055\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Recently, solid iron sources have been used for scorodite synthesis in arsenic-bearing wastewater from nonferrous metallurgy. Immobilising arsenic-solution as scorodite via iron hydroxide (Fe(OH)<sub>3</sub>) solid iron source is an important method for controlling arsenic pollution. The evolution behavior of scorodite during its formation in high arsenic solution have been rarely investigated. In this paper, the mechanism and kinetics of scorodite formation using Fe(OH)<sub>3</sub> in arsenic-bearing solution were investigated. This work was divided into three parts. Firstly, the influencing parameters were investigated, revealing that the dissolution of Fe(OH)<sub>3</sub> and scorodite generation accelerated at lower initial pH and higher reaction temperature. Increasing Fe/As ratio delayed scorodite crystallisation, which was in turn enhanced by elevating arsenic concentration. Secondly, the mechanism of scorodite formation was investigated, revealing that Fe(OH)<sub>3</sub> underwent acidic dissolution to form a precursor. Subsequent scorodite formation had a Δ<sub>r</sub>G<sub>m</sub><sup>θ</sup> ranging from −69.39 kJ·mol<sup>−1</sup> to −15.64 kJ·mol<sup>−1</sup>. Residual As was absorbed and converted into Fe(OH)<sub>3</sub>@scorodite. Thirdly, the chemical kinetics were investigated, showing that activation energy (Ea) for Fe(OH)<sub>3</sub> dissolution was 72.54 and 105.37 kJ·mol<sup>−1</sup> at Stages I and II, respectively, whereas it was 105.97 kJ·mol<sup>−1</sup> for residual As absorption-conversion at Stage III outweighing the Ea of As-Fe coprecipitation. The restrictive steps were Fe(OH)<sub>3</sub> dissolution and residual arsenic absorption-conversion. This proposed method can be applied for environment-friendly treatment of 10-40 g/L of arsenic-bearing industrial effluent for scorodite formation. Overall, this research confirmed the formation of scorodite via Fe(OH)<sub>3</sub> and can potentially provide feasible schemes for eliminating arsenic-bearing acidic waste, dust, and anode slime from nonferrous metallurgical processes.</p></div>\",\"PeriodicalId\":20743,\"journal\":{\"name\":\"Process Safety and Environmental Protection\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":6.9000,\"publicationDate\":\"2024-09-14\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Process Safety and Environmental Protection\",\"FirstCategoryId\":\"93\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0957582024011959\",\"RegionNum\":2,\"RegionCategory\":\"环境科学与生态学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Process Safety and Environmental Protection","FirstCategoryId":"93","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0957582024011959","RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
Mechanism and kinetics of scorodite formation in arsenic-bearing solutions using Fe(OH)3 as a solid iron source
Recently, solid iron sources have been used for scorodite synthesis in arsenic-bearing wastewater from nonferrous metallurgy. Immobilising arsenic-solution as scorodite via iron hydroxide (Fe(OH)3) solid iron source is an important method for controlling arsenic pollution. The evolution behavior of scorodite during its formation in high arsenic solution have been rarely investigated. In this paper, the mechanism and kinetics of scorodite formation using Fe(OH)3 in arsenic-bearing solution were investigated. This work was divided into three parts. Firstly, the influencing parameters were investigated, revealing that the dissolution of Fe(OH)3 and scorodite generation accelerated at lower initial pH and higher reaction temperature. Increasing Fe/As ratio delayed scorodite crystallisation, which was in turn enhanced by elevating arsenic concentration. Secondly, the mechanism of scorodite formation was investigated, revealing that Fe(OH)3 underwent acidic dissolution to form a precursor. Subsequent scorodite formation had a ΔrGmθ ranging from −69.39 kJ·mol−1 to −15.64 kJ·mol−1. Residual As was absorbed and converted into Fe(OH)3@scorodite. Thirdly, the chemical kinetics were investigated, showing that activation energy (Ea) for Fe(OH)3 dissolution was 72.54 and 105.37 kJ·mol−1 at Stages I and II, respectively, whereas it was 105.97 kJ·mol−1 for residual As absorption-conversion at Stage III outweighing the Ea of As-Fe coprecipitation. The restrictive steps were Fe(OH)3 dissolution and residual arsenic absorption-conversion. This proposed method can be applied for environment-friendly treatment of 10-40 g/L of arsenic-bearing industrial effluent for scorodite formation. Overall, this research confirmed the formation of scorodite via Fe(OH)3 and can potentially provide feasible schemes for eliminating arsenic-bearing acidic waste, dust, and anode slime from nonferrous metallurgical processes.
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