不同来源腐殖酸对三价锑的光氧化作用及影响因素

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Abstract

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^-、SO₄^2- 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.

Key words： humic acids photooxidation antimony free radical soil

Received: 30 June 2016

PACS:

X131

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	Articles by authors
	SUN Fu-hong
	PAN Feng-yun
	CHEN Yan-qing
	YAN Yuan-bo
	WU Feng-chang

Cite this article:

SUN Fu-hong,PAN Feng-yun,CHEN Yan-qing等. Photoxidation of antimony(III) and influencing factors in the presence of humic acids with different origins[J]. CHINA ENVIRONMENTAL SCIENCECE, 2016, 36(12): 3729-3736.

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http://manu36.magtech.com.cn/Jweb_zghjkx/EN/ OR http://manu36.magtech.com.cn/Jweb_zghjkx/EN/Y2016/V36/I12/3729

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[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.
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[19]	林樱,吴丰昌,白英臣,等.我国土壤和沉积物中富里酸标准样品的提取和表征[J].环境科学研究,2011,24(10):64-70.
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[22]	邱慧敏,耿金菊,韩超,等.亚磷酸盐在硝酸根溶液中的光氧化过程及影响因素[J].中国环境科学,2016,36(5):1442-1448.
[23]	邓亚运,庄英滢,冯越,等.顺硝烯新烟碱杀虫剂环氧虫啶在水中的光降解[J].中国环境科学,2016,36(4):1112-1118.
[1]	何孟常,季海冰,赵承易,等.锑矿区土壤和植物中重金属污染初探[J].北京师范大学学报:自然科学版,2002,38(3):417-420.
[2]	吴丰昌,郑建,潘响亮,等.锑的环境生物地球化学循环与效应研究展望[J].地球科学进展,2008,23(4):350-356.
[3]	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.
[4]	Shotyk W,Krachler M,Chen B.Antimony:Global environmental contaminant[J].J.Environ.Monitor.,2005,7:1135-1136.
[5]	戈兆凤,韦朝阳.锑环境健康效应的研究进展[J].环境与健康杂志,2011,28(7):649-653.
[6]	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.
[19]	林樱,吴丰昌,白英臣,等.我国土壤和沉积物中富里酸标准样品的提取和表征[J].环境科学研究,2011,24(10):64-70.
[20]	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.
[22]	邱慧敏,耿金菊,韩超,等.亚磷酸盐在硝酸根溶液中的光氧化过程及影响因素[J].中国环境科学,2016,36(5):1442-1448.
[23]	邓亚运,庄英滢,冯越,等.顺硝烯新烟碱杀虫剂环氧虫啶在水中的光降解[J].中国环境科学,2016,36(4):1112-1118.