Arsenic(As)removal from smelting acidic wastewater is an urgent task.The most common method is oxidation of trivalent As(III)to pentavalent As(V)subsequently precipitated by ferric(Fe(III))salts.Foundations of redox b...Arsenic(As)removal from smelting acidic wastewater is an urgent task.The most common method is oxidation of trivalent As(III)to pentavalent As(V)subsequently precipitated by ferric(Fe(III))salts.Foundations of redox behavior and chemical species are of great importance for understanding As removal.In this work,cyclic voltammetry(CV)and UV?Vis spectroscopy were used for laboratory observation;meanwhile HSC and MINTEQ software were employed for theoretical analyses.It is found that As(III)oxidation,a multiple electron transfer reaction,is diffusion-controlled.The oxidation over-potential is very high(about0.9V)in sulfuric acid solutions(pH1.0).In addition,Fe(III)?As(V)complexes are evidenced by UV?Vis spectra and chemical species analyses in series of Fe(III)?As(V)?H2SO4?H2O solutions.Therefore,the Fe(III)and As(V)species distribution against pH values are determined and a newφ?pH diagram with inclusion of Fe?As complexes is consequently compiled based on thermodynamic data predicted by other researchers.展开更多
Scorodite（FeAsO4·2H2O）is the most popular phase for arsenic（As）immobilization while the reductive dissolution of Fe（Ⅲ）to Fe（Ⅱ）will promote As release.In the present study,an equilibrium between Fe（Ⅲ）...Scorodite（FeAsO4·2H2O）is the most popular phase for arsenic（As）immobilization while the reductive dissolution of Fe（Ⅲ）to Fe（Ⅱ）will promote As release.In the present study,an equilibrium between Fe（Ⅲ）and Fe（Ⅱ）was achieved in scorodite preparation system by introducing certain alcohol（methanol,ethanol,isopropanol or tert-butanol）,and thus a new mixed-valent iron arsenate black crystal formulated as Fe（Ⅱ）（5.2）Fe（Ⅲ）（8.8）（HAsO4）4（AsO4）8·H2O was prepared.In comparison with scorodite,the black crystal has higher As content（36.4%,mass fraction）and lower crystal water content（0.73%,mass fraction）.Additionally,the leaching concentration of As can be lower than the threshold value（5 mg/L）regulated by identification standards for hazardous wastes of China（GB 5080.3-2007）.Therefore,this new mixed-valent iron arsenate crystal could be classified as a non-hazardous and promising As-bearing phase in environmental applications.展开更多
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,China
文摘Arsenic(As)removal from smelting acidic wastewater is an urgent task.The most common method is oxidation of trivalent As(III)to pentavalent As(V)subsequently precipitated by ferric(Fe(III))salts.Foundations of redox behavior and chemical species are of great importance for understanding As removal.In this work,cyclic voltammetry(CV)and UV?Vis spectroscopy were used for laboratory observation;meanwhile HSC and MINTEQ software were employed for theoretical analyses.It is found that As(III)oxidation,a multiple electron transfer reaction,is diffusion-controlled.The oxidation over-potential is very high(about0.9V)in sulfuric acid solutions(pH1.0).In addition,Fe(III)?As(V)complexes are evidenced by UV?Vis spectra and chemical species analyses in series of Fe(III)?As(V)?H2SO4?H2O solutions.Therefore,the Fe(III)and As(V)species distribution against pH values are determined and a newφ?pH diagram with inclusion of Fe?As complexes is consequently compiled based on thermodynamic data predicted by other researchers.
基金Project(51634010)supported by the Key Project of National Natural Science Foundation of ChinaProject(51304251)supported by the National Natural Science Foundation of ChinaProject(201509050)supported by Special Program on Environmental Protection for Public Welfare of China
文摘Scorodite（FeAsO4·2H2O）is the most popular phase for arsenic（As）immobilization while the reductive dissolution of Fe（Ⅲ）to Fe（Ⅱ）will promote As release.In the present study,an equilibrium between Fe（Ⅲ）and Fe（Ⅱ）was achieved in scorodite preparation system by introducing certain alcohol（methanol,ethanol,isopropanol or tert-butanol）,and thus a new mixed-valent iron arsenate black crystal formulated as Fe（Ⅱ）（5.2）Fe（Ⅲ）（8.8）（HAsO4）4（AsO4）8·H2O was prepared.In comparison with scorodite,the black crystal has higher As content（36.4%,mass fraction）and lower crystal water content（0.73%,mass fraction）.Additionally,the leaching concentration of As can be lower than the threshold value（5 mg/L）regulated by identification standards for hazardous wastes of China（GB 5080.3-2007）.Therefore,this new mixed-valent iron arsenate crystal could be classified as a non-hazardous and promising As-bearing phase in environmental applications.
