GeologicalScienceandTechnologyInformation Vol.37 No.5 Sep doi: /j.cnki.dzkq ,,,. [J].,2018,37(5): a,b a,b a,

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1 GeologicalScienceandTechnologyInformation Vol.37 No.5 Sep doi: /j.cnki.dzkq [J] (5): ab ab ab ab ( )a. ;b. 3007) : : ph Ec SO 2- HCO 3 - As / / : ; ; ; ; :X131.2 :A : (2018) [1-2] As [15-19] (Ⅲ) As(Ⅴ) [3-5] : [6] ; (SO 2- NO 3 - ) 1 [7-9] ; [10-12] km 2 - [13] [121] 00 mm 7 [20] - [21] - : : : (137225); (2016ACA167) : (1993 ) yanyijun 23@163.com : (1979 ) E- mail:cug xxj@163.com

5 : 207 2 (7 m 7 m) ( 1) 20.5~22.5 m 2 18.35~195μg/L 2.7~26.2 m Fig.2 Locationsofthemonitoringwels 25.67~33μg/L [20] 1018.7m DR2800 0.5μm 2m 0.20.0.611.52.03.

2 5 : (7 m 7 m) ( 1) 20.5~22.5 m ~195μg/L 2.7~26.2 m Fig.2 Locationsofthemonitoringwels 25.67~33μg/L [20] m DR μm 2m m TOC ( 2) ph 2 PW2 TOC Cl - SO 2- NO CompactIC Ca 2+ Mg 2+ Na + K + IRISIntrepid 2d IXSP ICP-AES As 2d 7d 11d AFS-9700 TOC 3 Picarro TOC-CRDS 8d ±5% [22] 60cm 2cm ; 60~200cm 5cm Thi [23] ( 1) ( ) ph ORP Ec (S 2- Fe 2+ NH -N NO 2 - ) ph 1 ORP Ec HACH HQ Table1 Paralelchemicalextractionprocedureforsolid- 0-d 2h phasearsenic HACH 1 0.5mol /L NaClpH=8 2 h mol /L ph=3 2 h mol /L ph=3 2h25 0.2mol /L +0.1mol/L ph=3 2h Fig.1 Locationofthestudysite 3.1 PW2 2m HCO 3-Na

208 2018 ( 3) HCO 3-0~2m 37.56mg/L Cl - SO 2- ( ) Ca 2+ 21.067mg/L Na + Cl - SO 2- HCO 3 - Na + 237.38mg/L Mg 2+ Ca 2+ Mg 2+ 18.828.92 mg/l PW2 ph 7.95-171.8 mv PW2 3.2 38μg/L 10μg/LAs(Ⅲ) 5-a 0.20. 79% 0.

3 ( 3) HCO 3-0~2m 37.56mg/L Cl - SO 2- ( ) Ca mg/L Na + Cl - SO 2- HCO 3 - Na mg/L Mg 2+ Ca 2+ Mg mg/l PW2 ph mv PW μg/L 10μg/LAs(Ⅲ) 5-a % 0.6m 591d μg/L m 0.5~2.0μg/L 0 ~2m 10μg/ L As(Ⅲ)/As T 5-b As(Ⅲ)/As T As(Ⅴ) As(Ⅲ) As 3 (Ⅲ)/As T Fig.3 Piperdiagramofsoilporewaterinirrigationareaand As(Ⅲ ) As(Ⅴ ) groundwaterofpumpingwels As(Ⅲ)/As T Cl-Na( 3) Cl - SO 2- HCO - 3 Na + Mg 2+ Ca 2+ (b) Fig.5 VariationofAsconcentrations(a)andAs(Ⅲ)/As Tratio Fig. Variationoftheaverageconcentrationsofmainionsin (b)ofsoilporewaterduringtheirrigationpractice soilporewatersamplesduringtheirrigation 5 (a) As(Ⅲ)/As T

4 5 : 209 0~2m 10μg/L 3 m Ec 1.2~5.79mS/ ( 2) cm ( 6-b) Ec 1.83μg/L 100μg/L As(Ⅲ) / As(Ⅴ ) As / [26] (Ⅲ)As(Ⅲ) 3 m 3m SO 2- HCO 3 - As(Ⅲ) HPO 2- [27-28] As(Ⅲ)/As T SO 2- HCO 3 - As (V) As(Ⅲ) ( 7) As(Ⅲ) As(Ⅴ) SO 2- HCO m As(Ⅲ) SO 2- HCO 3 - Table2 VariationofAsconcentrationsof3.0 m phreatic waterduringtheirrigation SO 2- SO 2- As(Ⅴ) As(Ⅲ) [29] S-0 S1 - S-2 S-3 S- S-5 S-6 S-7 SO 2- HCO As(Ⅲ) / As(Ⅴ) / As(Ⅲ)/AsT / [30] / / ρ (TOC) ρ (As) ( 8-a) ph 7.33 CO 2 ~8.79 HCO 3 - ( 6-a) ρ ( HCO 3 - ) ρ (TOC) ( [2-25] ph 8-b) ( 9-a) 6 ph (a) Ec (b) Fig.6 RelationshipbetweenAsconcentrationsversuspH (a)ec(b)ofsoilporewater

5 As(Ⅲ) As(Ⅴ) SO 2- HCO 3 - Fig.7 RelationshipsbetweenAs(Ⅲ) As(Ⅴ)concentrationsversusSO 2- HCO 3ofsoilporewater 8 TOC (a) HCO 3 - (b) Fig.8 RelationshipsbetweenTOCversusAsconcentrations(a)HCO - 3 (b)ofsoilporewater (Fe / (OH) 3 ) (FeOOH) 2O 3 ) SI

6 5 : (a) Fe(OH) 3 (b)fe(ooh)(c)fe 2O 3 (d) Fig.9 RelationshipsbetweenAsconcentrationsversusFeconcentrations(a)andtheSIofFe(OH) 3 (b)feooh(c)fe 2O 3 (d) ( 9-b~ d) 50%~62% ρ ( As) 3. ( 10) 5% 0~0.1m 11

２１２地质科技情报２０１８年图１０灌溉前后沉积物中总砷及各形态砷质量分数对比Ｆｉｇ１０Ｃｏｍｐａｒｉｓｏｎｏｆｄｉｆｆｅｒｅｎｔａｒｓｅｎｉｃｐｈａｓｅｓｏｆｓｅｄｉｍｅｎｔｓｂｅｆｏｒｅｔｈｅｉｒｒｉｇａｔｉｏｎａｎｄａｆｔｅｒｔｈｅｉｒｒｉｇａｔｉｏｎ图１１灌溉过程中非饱和带中砷的迁移转化机理Ｆｉｇ１１Ｓｃｈｅｍａｔｉｃｄｉａｇｒａｍ

7 ２１２地质科技情报２０１８年图１０灌溉前后沉积物中总砷及各形态砷质量分数对比Ｆｉｇ１０Ｃｏｍｐａｒｉｓｏｎｏｆｄｉｆｆｅｒｅｎｔａｒｓｅｎｉｃｐｈａｓｅｓｏｆｓｅｄｉｍｅｎｔｓｂｅｆｏｒｅｔｈｅｉｒｒｉｇａｔｉｏｎａｎｄａｆｔｅｒｔｈｅｉｒｒｉｇａｔｉｏｎ图１１灌溉过程中非饱和带中砷的迁移转化机理Ｆｉｇ１１Ｓｃｈｅｍａｔｉｃｄｉａｇｒａｍｏｆａｒｓｅｎｉｃｍｉｇｒａｔｉｏｎａｎｄｔｒａｎｓｆｏｒｍａｔｉｏｎｉｎｔｈｅｕｎｓａｔｕｒａｔｅｄｚｏｎｅｄｕｒｉｎｇｔｈｅｉｒｒｉｇａｔｉｏｎ为易被还原的无定形铁氧化物无定形铁氧化物进氧化物转化为无定形铁氧化物无定形铁氧化物以一步还原溶解以吸附共沉淀形式与之结合的砷被及碳酸盐铁溶解导致砷的释放但仍有Ｏ２进入近地表的非饱和带使Ｆｅ Ⅱ 被氧化为Ｆｅ Ⅲ 进而形成结晶态铁氧化物Ａｓ Ⅲ 被迅速氧化为Ａｓ Ⅴ 以吸附共沉淀形式被结晶态铁氧化物固定释放进入水体中同时部分碳酸盐铁也被溶解导致砷的释放被释放的Ａｓ Ⅴ 在还原环境下被还原为Ａｓ Ⅲ Ａｓ Ⅲ 的迁移性比Ａｓ Ⅴ 强很多生成的Ａｓ Ⅲ 向下迁移进入地下水中在接近地表的非饱和带灌溉使其还原环境变强存在部分结晶态铁灌溉结束后水回落大量Ｏ２进入土壤孔隙中导致土壤氧化性逐渐增强更多Ｆｅ Ⅱ 被氧化

8 5 : 213 Fe(Ⅲ) As(Ⅲ) bangladesh [J].Science :58. As(Ⅴ) / 5 (1) Cl-Na Cl - SO 2- HCO 3 - Na + Mg 2+ Ca 2+ 0~2m ogy (1): μg/L As(V) As(Ⅲ) 736. (2) ph Ec SO 2- HCO 3 - As / istry200520(10): (3) / As(V) As(Ⅲ) O 2 Fe(Ⅱ) Fe(Ⅲ) : [17]Polizzoto M LLinebergerE MMatesonA Retal.Arsenic transportinirrigation wateracrossrice-fieldsoilsinbangla- [1]. [J]. : (): (1): [19]DitmarJVoegelinARobertsLCetal.Arsenicaccumula- [2] MelikerJRWahlRLCameronLLetal.Arsenicindrinking tioninapaddyfieldin Bangladesh:Seasonaldynamicsand waterandcerebrovasculardiseasediabetesmelitusandkid- trendsoverathree-yearmonitoringperiod.[j].environmental neydiseasein Michigan:Astandardizedmortalityratioanalysis Science & Technology2010(8): [J].EnvironmentalHealth20076(1):. [3] Nordstrom D K.Publichealth:Worldwideoccurrencesofarse- nicingroundwater[j].science : []. [J] (11): [5] FendorfSMichaelH AGeenA V.Spatialandtemporalvaria- tionsofgroundwaterarsenicinsouthandsoutheastasia[j]. Science :1123. [6] BusbeeM WKocarBDBennerSG.Irrigationproducesele- vatedarsenicintheunderlyinggroundwaterofasemi-aridba- sininsouthwesternidaho[j].appliedgeochemistry20092 (5): [7] HarveyCFSwartzCBadruzzamanA B Metal.Responseto commentson arsenicmobilityandgroundwaterextractionin ence : [8] Harvey C FSwartzC HBadruzzaman A Betal.Arsenic mobilityandgroundwaterextractionin Bangladesh[J].Sci- [9] BuschmannJBerg M.Impactofsulfatereductiononthescale ofarseniccontaminationingroundwaterofthemekongben- galandredriverdeltas[j].appliedgeochemistry20092 (7): [10]HarveyCFAshfaqueK NYu Wetal.Groundwaterdynam- icsandarseniccontaminationinbangladesh[j].chemicalgeol- [11]NakayaSNatsumeHMasudaHetal.Efectofgroundwater flowonformingarseniccontaminatedgroundwaterinsonarga- onbangladesh[j].journalofhydrology201109(3):72- [12]XieXWangYSuCetal.Influenceofirrigationpracticeson arsenic mobilization:evidencefrom isotopecomposition and Cl/Brratiosingroundwaterfrom DatongBasinnorthernChi- na[j].journalofjinanuniversity20062/25(6):37-7. [1]XieXWangYElisAetal.Delineationofgroundwaterflow pathsusinghydrochemicalandstrontiumisotopecomposition: sinnorthernchina[j].journalofhydrology201376(2): [15]PanaulahG MAlam THossain M Betal.Arsenictoxicityto rice(oryzasatival.)inbangladesh[j].plant & Soil (1/2):31. [13]NorraSBernerZ AAgarwalaPetal.Impactofirrigation withasrichgroundwateronsoilandcrops:ageochemicalcase studyin WestBengalDeltaPlainIndia[J].AppliedGeochem- AcasestudyinhigharsenicaquifersystemsoftheDatongba- [16]Polizzoto M LKocarB DBennerS Getal.Near-surface wetlandsedimentsasasourceofarsenicreleasetogroundwa- terinasia.[j].nature20085: desh[j].environmentalpolution (179c):210. [18]. [J]. [20]. [J] (2): [21]. [J] (3): [22]. [D]. : ( )2008. plainatnam DuVietnam.[J].GeochimicaetCosmochimica Acta20112: [23]ThiH M NPostmaDThiK TPetal.Adsorptionandde- sorptionofarsenictoaquifersedimentontheredriverflood- [2] WaychunasG AReaB AFulerCCetal.Surfacechemistry offerrihydrite:part1.exafsstudiesofthegeometryofco- precipitatedandadsorbedarsenate[j].geochimicaetcosmo-

9 chimicaacta199357(10): [25]FrostR RGrifinR A.EfectofpHonadsorptionofarsenic andseleniumfromlandfilleachatebyclay minerals[j].soil ScienceSocietyofAmericaJournal19771(1): [26]MercerK LTobiasonJE.Removalofarsenicfromhighionic strengthsolutions:efectsofionicstrengthphand pre- formedversusinsituformed HFO[J].EnvironmentalScience & Technology20082(10): [27]ZhaoH SRS.Competitiveadsorptionofphosphateandarse- nateongoethite[j].environmentalscience & Technology (2): InfluenceofIrrigationPracticesonArsenicMobilization andtransformationintheunsaturatedzone YanYijun ab XieXianjun ab XiaoZiyi ab LiJunxia ab (a.schoolofenvironmentalstudies;b.statekeylaboratoryofbiogeologyand EnvironmentalGeologyChinaUniversityofGeosciences(Wuhan)Wuhan3007China) [28]RaduTSubaczJLJohnJ M Petal.Efectsofdissolved carbonateonarsenicadsorptionandmobility[j].environmen- talscience & Technology200539(20): [29]BurtonEDJohnstonSGBushR T.Microbialsulfidogenesis inferrihydrite-richenvironments:efectsoniron mineralogy andarsenic mobility[j].geochimicaetcosmochimica Acta (11): [30]XieXWangYElisAetal.Multipleisotope(OSandC) approachelucidatestheenrichmentofarsenicinthegroundwa- terfromthedatongbasinnorthernchina[j].journalofhy- drology201398(18): Abstract:Inthisstudytheinfluencemechanismofirrigationpracticesonarsenicmobilizationandtrans- formationintheunsaturatedzoneisdiscussedbyfieldirrigationpractices.theresultsshowthatarsenic mobilizationintheunsaturatedzoneduringhigharsenicgroundwaterirrigationpracticesisinfluencedby multiplegeochemicalprocess.thearsenicconcentrationisafectedbythephthecompetitiveadsorption betweenso 2- andhco 3 - andtheredoxvolatilityintheunsaturatedzone.duringtheirrigationthesoilis intherelativelyreducingconditionstheironoxidemineralisdissolvedandthearsenicwhichiscombined withtheironoxidemineralduetocoprecipitationorsorptionisreleasedintosoilporewater.aftertheirri- gationthesoilcomesintotherelativelyoxidizingconditionsinwhichtheironoxidemineralprecipitates andthearsenicofsoilpore waterisfixedbytheironoxide mineralduetocoprecipitationorsorption. Thereforethechangeoftheredoxconditionwhichcausestheprecipitation/dissolutionoftheironoxide mineralisthemainreasonofarsenicmobilizationintheunsaturatedzoneinirrigationpractices. Keywords:arsenic;irrigation;unsaturatedzone;adsorption;redox

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