Photoxidation of antimony(III) and influencing factors in the presence of humic acids with different origins
SUN Fu-hong1, PAN Feng-yun1, CHEN Yan-qing1,2, YAN Yuan-bo1, WU Feng-chang1
1. State Key Laboratory of Environmental Criteria and Risk Assessment, Chinese Research Academy of Environmental Sciences, Beijing 100012, China;
2. Environmental Standards Institute, Chinese Research Academy of Environmental Sciences, Beijing 100012, China
Antimony (Ⅲ) is the unstable reduced form involved in the biogeochemical cycling of toxic metals Sb. The photooxidation of Sb(Ⅲ) by humic acids may be the important means for environmental fates of Sb(Ⅲ) in aquatic ecosystem. In this study, the kinetic characteristics for Sb(Ⅲ) oxidation in the presence of humic acids with different origins were examined under photoirradiation. The photooxidation behaviors of Sb(Ⅲ) were investigated over a wide range of DOC concentrations, initial Sb(Ⅲ) concentrations, pH values and the occurrence of competitive ions. The mechanisms for the photoxidation of Sb(Ⅲ) by humic acids were discussed. The photooxidation of Sb(Ⅲ) by humic acids followed the pseudo-first-order kinetics model. The photooxidation rate constants increased rapidly with increasing pH values and DOC concentrations in the Sb(Ⅲ)-humic acids reaction systems. However, Sb(Ⅲ) photooxidation was inhibited with increasing initial Sb(Ⅲ) concentrations. The photooxidation rate constants of Sb(Ⅲ) under the humic acids with lignite origin were higher than that with soil origin. The occurrence of anionic NO3- enhanced the photooxidation of Sb(Ⅲ). However, there were no obvious effects of Cl-、SO42- and Na+ on Sb(Ⅲ) photooxidation. The ESR spectra suggest that hydroxyl radicals and superoxide free radicals induced by light are were reactive oxidants for Sb(Ⅲ) photooxidation. Hydroxyl radicals were the primary oxidants for Sb(Ⅲ) photooxidation under the acidic condition, and superoxide free radicals became the main photo-oxidants under the neutral and alkaline condition.
孙福红, 潘凤云, 陈艳卿, 鄢元波, 吴丰昌. 不同来源腐殖酸对三价锑的光氧化作用及影响因素[J]. 中国环境科学, 2016, 36(12): 3729-3736.
SUN Fu-hong, PAN Feng-yun, CHEN Yan-qing, YAN Yuan-bo, WU Feng-chang. Photoxidation of antimony(III) and influencing factors in the presence of humic acids with different origins. CHINA ENVIRONMENTAL SCIENCECE, 2016, 36(12): 3729-3736.
Nakamaru Y M,Sekine K.Sorption behavior of selenium and antimony in soils as a function of phosphate ion concentration[J].Soil Sci.Plant Nutr.,2008,54:332-341.
Filella M,Belzile N,Chen Y W.Antimony in the environment:A review focused on natural waters Ⅱ.Relevant solution chemistry[J].Earth-Sci.Rev.,2002,59:265-285.
[7]
Steelt S,Amarasiriwardena D,Xing B S.An investigation of inorganic antimony species and antimony associated with soil humic acid molar mass fractions in contaminated soils[J].Environ.Pollu.,2007,148:590-598.
[8]
Quentel F,Filella M,Elleouet C,et al.Kinetic studies on Sb (Ⅲ) oxidation by hydrogen peroxide in aqueous solution[J].Environ.Sci.Technol.,2004,38(10):2843-2848.
[9]
Leuz A,Johnson C A.Oxidation of Sb (Ⅲ) to Sb (V) by O2and H2O2in aqueous solutions[J].Geochim.Cosmochim.Acta,2005,69(5):1165-1172.
[10]
Xi J,He M,Wang K,et al.Adsorption of antimony (Ⅲ) on goethite in the presence of competitive anions[J].J.Geochem.Explor.,2013,132:201-208.
[11]
Belzile N,Chen Y,Wang Z.Oxidation of antimony (Ⅲ) by amorphous iron and manganese oxyhydroxides[J].Chem.Geol.,2001,174(4):379-387.
[12]
Buschmann J,Canonica S,Sigg L.Photoinduced oxidation of antimony (Ⅲ) in the presence of humic acid[J].Environ.Sci.Technol.,2005,39(14):5335-5341.
[13]
Leuz A K,Monch H,Johnson C A.Sorption of Sb (Ⅲ) and Sb (V) to goethite:Influence on Sb (Ⅲ) oxidation and mobilization[J].Environ.Sci.Technol.,2006,40(23):7277-7282.
[14]
Hu X Y,Kong L H,He M C.Kinetics and mechanism of photopromoted oxidative dissolution of antimony trioxide[J].Environ.Sci.Technol.,2014,48(24):14266-14272.
[15]
Kong L H,Hu X Y,He M C.Mechanisms of Sb (Ⅲ) Oxidation by Pyrite-Induced Hydroxyl Radicals and Hydrogen Peroxide[J].Environ.Sci.Technol.,2015,49(6):3499-3505.
[16]
Buschmann J,Sigg L.Antimony (Ⅲ) binding to humic substances:Influence of pH and type of humic acid[J].Environ.Sci.Technol.,2004,38:4535-4541.
[17]
Fendorf S,Michael H A,van Geen A.Spatial and temporal variations of groundwater arsenic in south and southeast Asia[J].Science,2010,328:1123-1127.
[18]
Liu G,Fernandez A,Cai Y.Complexation of arsenite with humic acid in the presence of ferric iron[J].Environ.Sci.Technol.,2011,45:3210-3216.
Xu L J,Chu W,Graham N.Sonophotolytic degradation of dimethyl phthalate without catalyst:analysis of the synergistic effect and modeling[J].Water.Res.,2013,47(6):1996-2004.
[21]
Tella M,Pokrovski G S.Antimony (V) complexing with O-bearing organic ligands in aqueous solution:an X-ray absorption fine structure spectroscopy and potentiometric study[J].Mineral.Mag.,2008,72:205-209.
Nakamaru Y M,Sekine K.Sorption behavior of selenium and antimony in soils as a function of phosphate ion concentration[J].Soil Sci.Plant Nutr.,2008,54:332-341.
Filella M,Belzile N,Chen Y W.Antimony in the environment:A review focused on natural waters Ⅱ.Relevant solution chemistry[J].Earth-Sci.Rev.,2002,59:265-285.
[7]
Steelt S,Amarasiriwardena D,Xing B S.An investigation of inorganic antimony species and antimony associated with soil humic acid molar mass fractions in contaminated soils[J].Environ.Pollu.,2007,148:590-598.
[8]
Quentel F,Filella M,Elleouet C,et al.Kinetic studies on Sb (Ⅲ) oxidation by hydrogen peroxide in aqueous solution[J].Environ.Sci.Technol.,2004,38(10):2843-2848.
[9]
Leuz A,Johnson C A.Oxidation of Sb (Ⅲ) to Sb (V) by O2and H2O2in aqueous solutions[J].Geochim.Cosmochim.Acta,2005,69(5):1165-1172.
[10]
Xi J,He M,Wang K,et al.Adsorption of antimony (Ⅲ) on goethite in the presence of competitive anions[J].J.Geochem.Explor.,2013,132:201-208.
[11]
Belzile N,Chen Y,Wang Z.Oxidation of antimony (Ⅲ) by amorphous iron and manganese oxyhydroxides[J].Chem.Geol.,2001,174(4):379-387.
[12]
Buschmann J,Canonica S,Sigg L.Photoinduced oxidation of antimony (Ⅲ) in the presence of humic acid[J].Environ.Sci.Technol.,2005,39(14):5335-5341.
[13]
Leuz A K,Monch H,Johnson C A.Sorption of Sb (Ⅲ) and Sb (V) to goethite:Influence on Sb (Ⅲ) oxidation and mobilization[J].Environ.Sci.Technol.,2006,40(23):7277-7282.
[14]
Hu X Y,Kong L H,He M C.Kinetics and mechanism of photopromoted oxidative dissolution of antimony trioxide[J].Environ.Sci.Technol.,2014,48(24):14266-14272.
[15]
Kong L H,Hu X Y,He M C.Mechanisms of Sb (Ⅲ) Oxidation by Pyrite-Induced Hydroxyl Radicals and Hydrogen Peroxide[J].Environ.Sci.Technol.,2015,49(6):3499-3505.
[16]
Buschmann J,Sigg L.Antimony (Ⅲ) binding to humic substances:Influence of pH and type of humic acid[J].Environ.Sci.Technol.,2004,38:4535-4541.
[17]
Fendorf S,Michael H A,van Geen A.Spatial and temporal variations of groundwater arsenic in south and southeast Asia[J].Science,2010,328:1123-1127.
[18]
Liu G,Fernandez A,Cai Y.Complexation of arsenite with humic acid in the presence of ferric iron[J].Environ.Sci.Technol.,2011,45:3210-3216.
Xu L J,Chu W,Graham N.Sonophotolytic degradation of dimethyl phthalate without catalyst:analysis of the synergistic effect and modeling[J].Water.Res.,2013,47(6):1996-2004.
[21]
Tella M,Pokrovski G S.Antimony (V) complexing with O-bearing organic ligands in aqueous solution:an X-ray absorption fine structure spectroscopy and potentiometric study[J].Mineral.Mag.,2008,72:205-209.
