Siderite tailings is a potentially cost-free iron(Fe)source for arsenic(As)fixation in hazardous arsenic-calcium residues(ACR)as stable scorodite.In this study,a pure siderite reagent was employed to investigate the m...Siderite tailings is a potentially cost-free iron(Fe)source for arsenic(As)fixation in hazardous arsenic-calcium residues(ACR)as stable scorodite.In this study,a pure siderite reagent was employed to investigate the mechanism and optimal conditions for As fixation in ACR via scorodite formation,while the waste siderite tailings were used to further demonstrate the cotreatment method.The cotreatment method starts with an introduction of sulfuric acid to the ACR for As extraction and gypsum precipitation,and is followed by the addition of H_(2)O_(2) to oxidize As(Ⅲ)in the extraction solutions and finalized by adding siderite with continuous air injection for scorodite formation.The dissolution-oxidation of siderite can slowly produce Fe(Ⅲ)to control aqueous As(V)-Fe(Ⅲ)precipitation supersaturation for continuous scorodite crystallization.Chemical analyses show that the extraction efficiency of As from the ACR reaches 94.55%,while the precipitation yield of extracted As via scorodite formation arrives at 99.63% and 99.47%,leading to fixation efficiency of 94.20% and 94.04% in terms of the total As in the ACR by using siderite reagent and tailings,respectively.The final solid products show desirable TCLP stability and long-term stability,meeting the requirement for safe storage(GB 5085.3-2007).XRD,FTIR,and TEM results reveal that such high stability is attributable to the formation of scorodite and the surface adsorption of As on the raw siderite and secondary maghemite.This innovative and economical application of siderite tailings for the treatment of hazardous ACR can be extended to the management of hydrometallurgical wastes.展开更多
A process was proposed for removing and stabilizing arsenic(As) from anode slime. The anode slime with high arsenic concentration was pretreated by circular alkaline leaching process. Then, the arsenic in the leaching...A process was proposed for removing and stabilizing arsenic(As) from anode slime. The anode slime with high arsenic concentration was pretreated by circular alkaline leaching process. Then, the arsenic in the leaching solution can be further precipitated as a form of scorodite crystalline(FeAsO4·2H2O). In the precipitating arsenic reaction, in which ferrous ions were oxidized by air gas, the effects of acidity(p H), reaction temperature, air flow rate, initial concentration of arsenic and initial molar ratio of Fe(II) to As(V) on arsenic precipitation were investigated. The results showed that sufficiently stable crystal scorodite could be achieved under the condition of initial arsenic concentration of 10 g/L, pH 3.0-4.0, Fe/As molar ratio of 1.5, the temperature of 80-95 °C, and the air flow rate higher than 120 L/h. Under the optimal condition, more than 78% of arsenic could be precipitated as a form of scorodite crystalline. The As leaching concentration of the precipitates was less than 2.0 mg/L and the precipitates may be considered to be safe for disposal.展开更多
To improve stability of scorodite,a method of simultaneous synthesis and in-situ coating of scorodite was proposed.Scorodite particles with polyhedral and raspberry-like morphologies were synthesized in an Fe(Ⅱ).As(...To improve stability of scorodite,a method of simultaneous synthesis and in-situ coating of scorodite was proposed.Scorodite particles with polyhedral and raspberry-like morphologies were synthesized in an Fe(Ⅱ).As(Ⅴ).H2O system at 90℃and pH 1.5 by blowing oxygen gas into the system.When the initial Fe/As molar ratio exceeded 1:1,a coating of sulfate-containing iron(hydr)oxides formed on the surfaces of scorodite particles during synthesis.To evaluate the leaching stability of synthesized scorodite samples,toxicity characteristic leaching procedure(TCLP)tests were conducted at pH 4.93 for 60 h,and long-term leaching tests were conducted for 30.40 d within a pH range of 5.40.10.88.The leaching results indicated that the release of arsenic from scorodite was noticeably postponed by the coating,and the average arsenic concentrations in the leaching solutions were as low as 0.12 mg/L in the TCLP tests and lower than 0.5 mg/L in the long-term leaching tests.展开更多
Scorodite (FeAsO_(4)·H_(2)O) is a common arsenic-bearing (As-bearing) iron mineral in nearsurface environments that could immobilize or store As in a bound state.In flooded soils,microbe induced Fe(Ⅲ) or As(Ⅴ) ...Scorodite (FeAsO_(4)·H_(2)O) is a common arsenic-bearing (As-bearing) iron mineral in nearsurface environments that could immobilize or store As in a bound state.In flooded soils,microbe induced Fe(Ⅲ) or As(Ⅴ) reduction can increase the mobility and bioavailability of As.Additionally,humic substances can act as electron shuttles to promote this process.The dynamics of As release and diversity of putative As(Ⅴ)-reducing bacteria during scorodite reduction have yet to be investigated in detail in flooded soils.Here,the microbial reductive dissolution of scorodite was conducted in an flooded soil in the presence of anthraquinone-2,6-disulfonate (AQDS).Anaeromyxobacter,Dechloromonas,Geothrix,Geobacter,Ideonella,and Zoogloea were found to be the dominant indigenous bacteria during Fe(Ⅲ) and As(Ⅴ) reduction.AQDS increased the relative abundance of dominant species,but did not change the diversity and microbial community of the systems with scorodite.Among these bacteria,Geobacter exhibited the greatest increase and was the dominant Fe(Ⅲ)-and As(Ⅴ)-reducing bacteria during the incubation with AQDS and scorodite.AQDS promoted both Fe(Ⅲ) and As(Ⅴ) reduction,and over 80%of released As(Ⅴ) was microbially transformed to As(Ⅲ).The increases in the abundance of arrA gene and putative arrA sequences of Geobacter were higher with AQDS than without AQDS.As a result,the addition of AQDS promoted microbial Fe(Ⅲ) and As(Ⅴ) release and reduction from As-bearing iron minerals into the environment.These results contribute to exploration of the transformation of As from As-bearing iron minerals under anaerobic conditions,thus providing insights into the bioremediation of As-contaminated soil.展开更多
Arsenic-contained acid polymetallic solutions(AAPS)are produced from the H2SO4 leaching of dust generated during nonferrous metals pyrometallurgy such as copper,lead,and zinc.It is difficult to selectively remove As a...Arsenic-contained acid polymetallic solutions(AAPS)are produced from the H2SO4 leaching of dust generated during nonferrous metals pyrometallurgy such as copper,lead,and zinc.It is difficult to selectively remove As and efficiently recover valuable metals simultaneously.In this study,arsenic was removed from an acid polymetallic solution containing As,Cd,and Zn via scorodite formation using a hydrothermal method.First,a thermodynamic analysis of the Cd^(2+)-Zn^(2+)-Fe^(3+)-AsO_(4)^(3−)-SO_(4)^(2−)-H_(2)O system showed that the pH range for selective As removal as FeAsO4 was 1.8−3.9,and a higher pH will result in the precipitation of Cd in the form of Cd_(5)H_(2)(AsO_(4))_(4).Second,the experimental investigations,including neutralization and hydrothermal processes,showed that 88.96%As was selectively removed as scorodite with a flower cluster morphology in a hydrothermal process after adjusting the pH of AAPS to 1.0 via a neutralization process,while the total loss ratios of Cd and Zn were 2.44%and 1.13%,respectively.This study realized selective separation of Zn and Cd from AAPS by controlling the pH to avoid their loss into scorodite.展开更多
基金supported by the National Natural Science Foundation of China(Nos.42207258 and 52270150)the Liaoning Provincial Natural Science Foundation Program Project(No.2022-BS-312)+1 种基金the Liaoning University of Technology Doctoral Research Start-up Fund Project(No.XB2021013)the Shenyang Youth Science and Technology Project(No.RC210166).
文摘Siderite tailings is a potentially cost-free iron(Fe)source for arsenic(As)fixation in hazardous arsenic-calcium residues(ACR)as stable scorodite.In this study,a pure siderite reagent was employed to investigate the mechanism and optimal conditions for As fixation in ACR via scorodite formation,while the waste siderite tailings were used to further demonstrate the cotreatment method.The cotreatment method starts with an introduction of sulfuric acid to the ACR for As extraction and gypsum precipitation,and is followed by the addition of H_(2)O_(2) to oxidize As(Ⅲ)in the extraction solutions and finalized by adding siderite with continuous air injection for scorodite formation.The dissolution-oxidation of siderite can slowly produce Fe(Ⅲ)to control aqueous As(V)-Fe(Ⅲ)precipitation supersaturation for continuous scorodite crystallization.Chemical analyses show that the extraction efficiency of As from the ACR reaches 94.55%,while the precipitation yield of extracted As via scorodite formation arrives at 99.63% and 99.47%,leading to fixation efficiency of 94.20% and 94.04% in terms of the total As in the ACR by using siderite reagent and tailings,respectively.The final solid products show desirable TCLP stability and long-term stability,meeting the requirement for safe storage(GB 5085.3-2007).XRD,FTIR,and TEM results reveal that such high stability is attributable to the formation of scorodite and the surface adsorption of As on the raw siderite and secondary maghemite.This innovative and economical application of siderite tailings for the treatment of hazardous ACR can be extended to the management of hydrometallurgical wastes.
基金Projects(51304251,51374237)supported by the National Natural Science Foundation of ChinaProject(201509050)supported by Special Program on Environmental Protection for Public Welfare,ChinaProjects(2012FJ1010,2014FJ1011)supported by the Key Projects of Science and Technology of Hunan Province,China
文摘A process was proposed for removing and stabilizing arsenic(As) from anode slime. The anode slime with high arsenic concentration was pretreated by circular alkaline leaching process. Then, the arsenic in the leaching solution can be further precipitated as a form of scorodite crystalline(FeAsO4·2H2O). In the precipitating arsenic reaction, in which ferrous ions were oxidized by air gas, the effects of acidity(p H), reaction temperature, air flow rate, initial concentration of arsenic and initial molar ratio of Fe(II) to As(V) on arsenic precipitation were investigated. The results showed that sufficiently stable crystal scorodite could be achieved under the condition of initial arsenic concentration of 10 g/L, pH 3.0-4.0, Fe/As molar ratio of 1.5, the temperature of 80-95 °C, and the air flow rate higher than 120 L/h. Under the optimal condition, more than 78% of arsenic could be precipitated as a form of scorodite crystalline. The As leaching concentration of the precipitates was less than 2.0 mg/L and the precipitates may be considered to be safe for disposal.
基金Project(51574285)supported by the National Natural Science Foundation of China
文摘To improve stability of scorodite,a method of simultaneous synthesis and in-situ coating of scorodite was proposed.Scorodite particles with polyhedral and raspberry-like morphologies were synthesized in an Fe(Ⅱ).As(Ⅴ).H2O system at 90℃and pH 1.5 by blowing oxygen gas into the system.When the initial Fe/As molar ratio exceeded 1:1,a coating of sulfate-containing iron(hydr)oxides formed on the surfaces of scorodite particles during synthesis.To evaluate the leaching stability of synthesized scorodite samples,toxicity characteristic leaching procedure(TCLP)tests were conducted at pH 4.93 for 60 h,and long-term leaching tests were conducted for 30.40 d within a pH range of 5.40.10.88.The leaching results indicated that the release of arsenic from scorodite was noticeably postponed by the coating,and the average arsenic concentrations in the leaching solutions were as low as 0.12 mg/L in the TCLP tests and lower than 0.5 mg/L in the long-term leaching tests.
基金supported by the National Science Foundation of China(Nos.41977291 and 42177238)the Science and Technology Foundation of Guangdong,China (Nos.2019A1515011482 and2022A1515011093)+2 种基金the Strategic Priority Research Program (No.XDB40020300)the GDAS’Project of Science and Technology Development (Nos.2019GDASYL-0102002-5 and2020GDASYL-20200103077)Light of West China of Chinese Academy of Sciences。
文摘Scorodite (FeAsO_(4)·H_(2)O) is a common arsenic-bearing (As-bearing) iron mineral in nearsurface environments that could immobilize or store As in a bound state.In flooded soils,microbe induced Fe(Ⅲ) or As(Ⅴ) reduction can increase the mobility and bioavailability of As.Additionally,humic substances can act as electron shuttles to promote this process.The dynamics of As release and diversity of putative As(Ⅴ)-reducing bacteria during scorodite reduction have yet to be investigated in detail in flooded soils.Here,the microbial reductive dissolution of scorodite was conducted in an flooded soil in the presence of anthraquinone-2,6-disulfonate (AQDS).Anaeromyxobacter,Dechloromonas,Geothrix,Geobacter,Ideonella,and Zoogloea were found to be the dominant indigenous bacteria during Fe(Ⅲ) and As(Ⅴ) reduction.AQDS increased the relative abundance of dominant species,but did not change the diversity and microbial community of the systems with scorodite.Among these bacteria,Geobacter exhibited the greatest increase and was the dominant Fe(Ⅲ)-and As(Ⅴ)-reducing bacteria during the incubation with AQDS and scorodite.AQDS promoted both Fe(Ⅲ) and As(Ⅴ) reduction,and over 80%of released As(Ⅴ) was microbially transformed to As(Ⅲ).The increases in the abundance of arrA gene and putative arrA sequences of Geobacter were higher with AQDS than without AQDS.As a result,the addition of AQDS promoted microbial Fe(Ⅲ) and As(Ⅴ) release and reduction from As-bearing iron minerals into the environment.These results contribute to exploration of the transformation of As from As-bearing iron minerals under anaerobic conditions,thus providing insights into the bioremediation of As-contaminated soil.
基金Project(23B05465) supported by the Scientific Research Fund of Hunan Provincial Education Department,China。
文摘Arsenic-contained acid polymetallic solutions(AAPS)are produced from the H2SO4 leaching of dust generated during nonferrous metals pyrometallurgy such as copper,lead,and zinc.It is difficult to selectively remove As and efficiently recover valuable metals simultaneously.In this study,arsenic was removed from an acid polymetallic solution containing As,Cd,and Zn via scorodite formation using a hydrothermal method.First,a thermodynamic analysis of the Cd^(2+)-Zn^(2+)-Fe^(3+)-AsO_(4)^(3−)-SO_(4)^(2−)-H_(2)O system showed that the pH range for selective As removal as FeAsO4 was 1.8−3.9,and a higher pH will result in the precipitation of Cd in the form of Cd_(5)H_(2)(AsO_(4))_(4).Second,the experimental investigations,including neutralization and hydrothermal processes,showed that 88.96%As was selectively removed as scorodite with a flower cluster morphology in a hydrothermal process after adjusting the pH of AAPS to 1.0 via a neutralization process,while the total loss ratios of Cd and Zn were 2.44%and 1.13%,respectively.This study realized selective separation of Zn and Cd from AAPS by controlling the pH to avoid their loss into scorodite.
