机构地区:[1]College of Resources and Environment, Huazhong Agricultural University, Wuhan 430070, China [2]College of Resources and Environment, Yunnan Agricultural University, Kunming 650201, China
出 处:《Journal of Environmental Sciences》2006年第2期292-298,共7页环境科学学报(英文版)
基 金:TheNationalN aturalScienceFoundationofChina (No.40471070;40403009)andtheK eyResearchProjectofM inistryofEducation,China(N o.105122)
摘 要:Oxidation of As(Ⅲ) by three types of manganese oxides and the effects ofpH, ion strength and tartaric acid on the oxidation were investigated by means of chemical analysis, equilibrium redox, X-ray diffraction (XRD) and transmission electron microscopy (TEM). Three synthesized Mn oxide minerals, bimessite, cryptomelane, and hausmannite, which widely occur in soil and sediments, could actively oxidize As(Ⅲ) to As(Ⅴ). However, their ability in As(Ⅲ)-oxidation varied greatly depending on their structure, composition and surface properties. Tunnel structured cryptomelane exhibited the highest ability of As (Ⅲ) oxidation, followed by the layer structured birnessite and the lower oxide hausmannite. The maximum amount of As (Ⅴ) produced by the oxidation was in the order (mmol/kg) of cryptomelane (824.2) 〉 bimessite (480.4) 〉 hausmannite (117.9), As pH increased from the very low value(pH 2.5), the amount of As(Ⅲ) oxidized by the tested Mn oxides was firstly decreased, then negatively peaked in pH 3.0 6.5, and eventually increased remarkably. Oxidation of As(Ⅲ) by the Mn oxides had a buffering effects on the pH variation in the solution. It is proposed that the oxidative reaction processes between As (Ⅲ) and biruessite(or cryptomelane) are as follows: (1) at lower pH condition: (MnO2)x+ H3AsO3 + 0.5H^+=0.5H2AsO4^- + 0.5HAsO4^2- +Mn〉^2+ (MnO2)x-1 + H2O; (2) at higher pH condition: (MnO2)x + H3AsO3 = 0.5H2AsO4^- + 0.5HAsO4^2- + 1.5H^+ + (MnO2)x-1. MnO. With increase of ion strength, the As(Ⅲ) oxidized by bimessite and cryptomelane decreased and was negatively correlated with ion strength. However, ion strength had little influence on As (Ⅲ) oxidation by the hausmarmite. The presence of tartaric acid promoted oxidation of As(Ⅲ) by birnessite. As for cryptomelane and hansmannite, the same effect was observed when the concentration of tartaric acid was below 4 mmolOxidation of As(Ⅲ) by three types of manganese oxides and the effects ofpH, ion strength and tartaric acid on the oxidation were investigated by means of chemical analysis, equilibrium redox, X-ray diffraction (XRD) and transmission electron microscopy (TEM). Three synthesized Mn oxide minerals, bimessite, cryptomelane, and hausmannite, which widely occur in soil and sediments, could actively oxidize As(Ⅲ) to As(Ⅴ). However, their ability in As(Ⅲ)-oxidation varied greatly depending on their structure, composition and surface properties. Tunnel structured cryptomelane exhibited the highest ability of As (Ⅲ) oxidation, followed by the layer structured birnessite and the lower oxide hausmannite. The maximum amount of As (Ⅴ) produced by the oxidation was in the order (mmol/kg) of cryptomelane (824.2) 〉 bimessite (480.4) 〉 hausmannite (117.9), As pH increased from the very low value(pH 2.5), the amount of As(Ⅲ) oxidized by the tested Mn oxides was firstly decreased, then negatively peaked in pH 3.0 6.5, and eventually increased remarkably. Oxidation of As(Ⅲ) by the Mn oxides had a buffering effects on the pH variation in the solution. It is proposed that the oxidative reaction processes between As (Ⅲ) and biruessite(or cryptomelane) are as follows: (1) at lower pH condition: (MnO2)x+ H3AsO3 + 0.5H^+=0.5H2AsO4^- + 0.5HAsO4^2- +Mn〉^2+ (MnO2)x-1 + H2O; (2) at higher pH condition: (MnO2)x + H3AsO3 = 0.5H2AsO4^- + 0.5HAsO4^2- + 1.5H^+ + (MnO2)x-1. MnO. With increase of ion strength, the As(Ⅲ) oxidized by bimessite and cryptomelane decreased and was negatively correlated with ion strength. However, ion strength had little influence on As (Ⅲ) oxidation by the hausmarmite. The presence of tartaric acid promoted oxidation of As(Ⅲ) by birnessite. As for cryptomelane and hansmannite, the same effect was observed when the concentration of tartaric acid was below 4 mmol
关 键 词:oxidation of As(Ⅲ) As(Ⅴ) Mn oxides pH ion strength tartaric acid
分 类 号:X131[环境科学与工程—环境科学]
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