Skip to main content
SpringerLink
Log in

Redox processes and occurrence of arsenic in a volcanic aquifer system of Kumamoto Area, Japan

  • Original Article
  • Published:
Environmental Earth Sciences Aims and scope Submit manuscript

Abstract

Sources, distributions, and controlling factors for mobilization of arsenic (As) in Kumamoto basin were investigated relating to the determination of redox processes of the study area. Groundwater and sediment core samples were analyzed. Nitric acid digestion and sequential leaching experiment of sediment core samples revealed that the source of As in the groundwater is geogenic and leached primarily due to the sediment–water interactions. Unlikely, similar relations of total As with total Fe, Mn, and Al in acid extracts, leaching experiments showed a positive relation of Astotal with Fetotal and Altotal indicated that Fe and Al oxides/hydroxides are abundant and may be the major adsorbent of As in low pH condition. Arsenic concentrations in groundwater ranges from 0.1 to 60.6 μg/l. High As concentrations occurred in anaerobic stagnant groundwaters from Kumamoto plain area with high dissolved Fetotal, Mntotal, and Altotal, moderately dissolved HCO3 −, PO4 3−, SO4 2−, and low concentrations of NO3 − and DOC suggesting the reducing condition of subsurface aquifer. There is a range of As(III)/As(T) ratios from mostly arsenate to mostly arsenite. Groundwater pH was relatively high, and high As occurred at higher pH range. It is assumed that desorption of As from metal oxide surfaces was facilitated by the elevated pH, which is considered as an important process for As mobilization. In addition to this, a wide range of δ34SSO4 values (8.3–57.6 ‰) indicates that sulfur is undergoing redox cycling mediated by microbial activities. Following δ34SSO4 results, it is anticipated that dissolved As is coprecipitated as sulfides in the presence of dissolved Fe(II) in some places, though at this moment, there is no direct evidence of coprecipitation or sequester of As with Fe and sulfide ion. Finally, a combination of the following three variables are considered potentially important causes for the high dissolved As concentrations in groundwater of Kumamoto area—(1) high groundwater pH, (2) anoxic redox conditions, and (3) stagnant groundwater in younger age sediments, which have not been well flushed since burial.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7
Fig. 8
Fig. 9
Fig. 10
Fig. 11

Similar content being viewed by others

References

  • Andersson A, Nilson A, Hakansson L (1991) Metal concentration of the mor layer. Swedish Environmental Protection Agency (SNV) report no. 3990, p 85

  • Bednar AJ, Garbarino JR, Ranville JF, Wildeman TR (2002) Preserving the distribution of inorganic arsenic species in groundwater and acid mine drainage samples. Environ Sci Technol 36(10):2213–2218

    Article  Google Scholar 

  • Bednar AJ, Garbarino JR, Burkhardt MR, Ranville JF, Wildeman TR (2004) Field and laboratory arsenic speciation methods and their application to natural-water analysis. Water Res 38(2):355–364

    Article  Google Scholar 

  • Berner R (1981) A new geochemical classification of sedimentary environments. J Sed Petrol 51:359–365

    Google Scholar 

  • Bhattacharya P, Jacks G, Jana J, Sracek A, Gustafsson JP, Chatterjee D (2001) Geochemistry of the Holocene alluvial sediments of Bengal delta plain from West Bengal, India: implications on arsenic contamination in groundwater. In: Jacks G, Bhattacharya P, Khan AA (eds) Groundwater arsenic contamination in the Bengal Delta Plain of Bangladesh, KTH Special Publication. TRITA-AMI Report 3084, pp 21–40

  • Bhattacharya P, Jacks G, Ahmed KM, Khan AA, Routh J (2002) Arsenic in groundwater of the Bengal delta plain aquifers in Bangladesh. Bull Environ Contam Toxicol 69:538–545

    Article  Google Scholar 

  • Bhattacharya P, Claesson M, Bundschuh J, Sracek O, Fagerberg J, Jacks G, Martin RA, Storniolo ADR, Thir JM (2006) Distribution and mobility of arsenic in the Rio Dulce alluvial aquifers in Santiago del Estero Province, Argentina. Sci Total Environ 358(1):97–120

    Article  Google Scholar 

  • Brookins DG (1988) Eh-pH diagrams for geochemistry. Springer, New York

    Book  Google Scholar 

  • Champ DR, Gulens J, Jackson RE (1979) Oxidation-reduction sequences in ground water flow systems. Can J Earth Sci 16(1):12–23

    Article  Google Scholar 

  • Chapelle FH, McMahon PB, Dubrovsky NM, Fujii RF, Oaksford ET, Vroblesky DA (1995) Deducing the distribution of terminal electron-accepting processes in hydrologically diverse groundwater systems. Water Resour Res 31(2):359–371

    Article  Google Scholar 

  • Chapelle FH, Bradley PM, Thomas MA, McMahon PB (2009) Distinguishing iron-reducing from sulfate-reducing conditions. Groundwater 47(2):300–305

    Article  Google Scholar 

  • De Vitre R, Belzile N, Tessier A (1991) Speciation and adsorption of arsenic on diagenetic iron oxyhydroxides. Limnol Oceanog 36:1480–1485

    Article  Google Scholar 

  • Dzombak DA, Morel FMM (1990) Surface complexation modelling—hydrous ferric oxide. Wiley, New York

    Google Scholar 

  • Gallagher PA, Schwegel CA, Wei X, Creed JT (2001) Speciation and preservation of inorganic arsenic in drinking water sources using EDTA with IC separation and ICP-MS detection. J Environ Monit 3(4):371–376

    Article  Google Scholar 

  • Garbarino JR, Bednar AJ, Burkhardt MR (2002) Methods of analysis by the US geological survey national water quality laboratory—arsenic speciation in natural-water samples using laboratory and field methods. US Geological Survey Water-Resources Investigations Report 02-4144

  • Guo T, DeLaune RD, Patrick WH (1997) The influence of sediment redox chemistry on chemically active forms of arsenic, cadmium, chromium, and zinc in estuarine sediment. Environ Int 23(3):305–316

    Article  Google Scholar 

  • Harvey CF, Swartz CH, Badruzzaman ABM, Keon-Blute N, Yu W, Ali MA, Jay J, Beckie R, Niedan V, Brabander D, Oates PM, Ashfaque KN, Islam S, Hemond HF, Ahmed MF (2002) Arsenic mobility and groundwater extraction in Bangladesh. Science 298:1602–1606

    Article  Google Scholar 

  • Hinkle SR, Polette DJ (1999) Arsenic in ground water of the Willamette Basin, Oregon. US Dept. of the Interior, US Geological Survey. http://hdl.handle.net/1957/5064. Accessed 15 June 2015

  • Hosono T, Tokunaga T, Kagabu M, Nakata H, Orishikida T, Lin IT, Shimada J (2013) The use of δ15N and δ18O tracers with an understanding of groundwater flow dynamics for evaluating the origins and attenuation mechanisms of nitrate pollution. Water Res 47:2661–2675

    Article  Google Scholar 

  • Hosono T, Tokunaga T, Tsusima A, Shimada J (2014) Use of δ13C, δ15N and δ34S to study anaerobic bacterial processes in groundwater flow systems. Water Res 54:284–296

    Article  Google Scholar 

  • Hossain S, Hosono T, Tokunaga T, Ide K, Shimada J (2013) Geochemical modeling of groundwater evolution in a volcanic aquifer system of Kumamoto area, Japan. In: American Geophysical Union (AGU) 2013 Fall Meeting, San Francisco, 9–13 December. Abstract H11H-1247

  • Hunter AG (1998) Intracrustal controls on the coexistence of tholeiitic and calc-alkaline magma series at Aso Volcano, SW Japan. J Petrol 39:1255–1284

    Article  Google Scholar 

  • Kent DB, Niedan VW, Isenbeck-Scrötter M, Stadler S, Jann S, Höhn R, Davies JA (2003) The influence of oxidation, reduction and adsorption reactions on arsenic transport in the oxic, suboxic and anoxic zones of a mildly acidic sand and gravel aquifer. http://wwwbrr.cr.usgs.gov/projects/GWC_chemtherm/FinalAbsPDF/kent.pdf. Accessed 2 May 2015

  • Kinniburgh DG, Jackson ML, Syers JK (1976) Adsorption of alkaline earth, transition, and heavy metal cations by hydrous oxide gels of iron and aluminum, Soil Sci. Soc Am J 40:796–799

    Article  Google Scholar 

  • Kirk MF, Holm TR, Park J, Jin Q, Sanford RA, Fouke BW et al (2004) Bacterial sulfate reduction limits natural arsenic contamination in groundwater. Geology 32:953–956

    Article  Google Scholar 

  • Kondo H, Ishiguro Y, Ohno K, Nagase M, Toba M, Takagi M (1999) Naturally occurring arsenic in the groundwaters in the southern region of Fukuoka Prefecture, Japan. Water Res 33(8):1967–1972

    Article  Google Scholar 

  • Kumamoto City Waterworks and Sewerage Bureau (2008) Annual report of water quality test, Kumamoto City, pp 246 (in Japanese)

  • Kumamoto Prefecture and Kumamoto City (1995) Integrated groundwater survey report of the Kumamoto Area, Kumamoto Prefecture and Kumamoto City, pp 122 (in Japanese)

  • Langmuir D (1997) Aqueous environmental geochemistry. Prentice-Hall, Upper Saddle River

    Google Scholar 

  • Langmuir D, Chrostowski P, Vigneault B, Chaney R (2005) Issue paper on the environmental chemistry of metals. US EPA Risk Assessment Forum, p A39

  • Lindberg RD, Runnells DD (1984) Ground water redox reactions: an analysis of equilibrium state applied to Eh measurements and geochemical modeling. Science 225:925–927

    Article  Google Scholar 

  • Luther GW, Sundby B, Lewis BL, Brendel PJ, Silverberg N (1997) Interactions of Manganese with the Nitrogen cycle: alternative pathways to Dinitrogen. Geochim Cosmochim Acta 61(19):4043–4052

    Article  Google Scholar 

  • Mason B, Moore CB (1982) Principles of geochemistry, 4th edn. Wiley, Hongkong

    Google Scholar 

  • McArthur JM (1999) Arsenic poisoning in the Ganges delta-Reply. Nature 401(6753):546–547

    Article  Google Scholar 

  • McArthur JM, Ravenscroft P, Safiullah S, Thirlwall MF (2001) Arsenic in groundwater: testing pollution mechanisms for sedimentary aquifers in Bangladesh. Water Resour Res 37:109–117

    Article  Google Scholar 

  • McArthur JM, Banerjee DM, Hudson-Edwards KA, Mishra R, Purohit R, Ravenscroft P, Cronin A, Howarth RJ, Chatterjee A, Talukder T, Lowry D, Houghton S, Chadha D (2004) Natural organic matter in sedimentary basins and its relation to arsenic in anoxic groundwater: the example of West Bengal and its worldwide implications. Appl Geochem 19:1255–1293

    Article  Google Scholar 

  • McMahon PB, Chapelle FH (2008) Redox processes and water quality of selected principal aquifer systems. Groundwater 46(2):259–271

    Article  Google Scholar 

  • Meng X, Korfiatis GP, Bang S, Bang KW (2002) Combined effects of anions on arsenic removal by iron hydroxides. Toxicol Lett 133(1):103–111

    Article  Google Scholar 

  • Nickson R, McArthur J, Burgess W, Ahmed KM, Ravenscorft P, Rahman M (1998) Arsenic poisoning of Bangladesh groundwater. Nature 395(6700):338

    Article  Google Scholar 

  • Nickson RT, McArthur JM, Ravenscroft P, Burgess WG, Ahmed KM (2000) Mechanism of arsenic release to groundwater, Bangladesh and West Bengal. Appl Geochem 15:403–413

    Article  Google Scholar 

  • Nordstrom DK (2002) Worldwide occurrences of arsenic in ground water. Science (Washington) 296(5576):2143–2145

    Article  Google Scholar 

  • Ottley CJ, Davison W, Edmunds WM (1997) Chemical catalysis of nitrate reduction by iron (II). Geochim Cosmochim Acta 61(9):1819–1828

    Article  Google Scholar 

  • Parkhurst DL, Appelo CAJ (1999) User’s guide to PHREEQC (Version 2)—a computer program for speciation, batch-reaction, one-dimensional transport, and inverse geochemical calculations: US Geological Survey Water-Resources Investigations Report 99-4259, p 312

  • Parkhurst DL, Christenson SC, Breit GN (1993) Ground-water-quality assessment of the central Oklahoma Aquifer, Oklahoma; geochemical and geohydrologic investigations Report No. 92-642, US Geological Survey; Books and Open-File Reports Section [distributor]

  • Robertson FN (1989) Arsenic in groundwater under oxidizing conditions, south-west United States. Environ Geochem Health 11:171–185

    Article  Google Scholar 

  • Smedley PL, Kinniburgh DG (2002) A review of the source, behaviour and distribution of arsenic in natural waters. Appl Geochem 17:517–568

    Article  Google Scholar 

  • Smedley PL, Zhang M, Zhang G, Luo Z (2003) Mobilisation of arsenic and other trace elements in fluviolacustrine aquifers of the Huhhot Basin, Inner Mongolia. Appl Geochem 18(9):1453–1477

    Article  Google Scholar 

  • Straub KL, Benz M, Schink B, Widdel F (1996) Anaerobic, nitrate-dependent microbial oxidation of ferrous iron. Appl Environ Microbiol 62(4):1458–1460

    Google Scholar 

  • Stüben D, Berner Z, Chandrasekharam D, Karmakar J (2003) Arsenic enrichment in groundwater of West Bengal, India: geochemical evidence for mobilization of As under reducing conditions. Appl Geochem 18(9):1417–1434

    Article  Google Scholar 

  • Stumm W, Morgan JJ (1996) Aquatic chemistry. Wiley, New York, p 780

    Google Scholar 

  • Su C, Puls RW (2003) In situ remediation of arsenic in simulated groundwater using zerovalent iron: laboratory column tests on combined effects of phosphate and silicate. Environ Sci Technol 37(11):2582–2587

    Article  Google Scholar 

  • Suess E, Wallschlager D, Planer-Friedrich B (2011) Stabilization of Thioarsenates in Iron-rich waters. Chemosphere 83(11):1524–1531

    Article  Google Scholar 

  • Sullivan KA, Aller RC (1996) Diagenetic cycling of arsenic in Amazon shelf sediments. Geochim Cosmochim Acta 60:1465–1477

    Article  Google Scholar 

  • Swartz CH, Blute NK, Badruzzaman B, Ali A, Brabander D, Jay J, Besancon J, Islam S, Hemond HF, Harvey CF (2004) Mobility of arsenic in a Bangladesh aquifer: inferences from geochemical profiles, leaching data, and mineralogical characterization. Geochim Cosmochim Acta 68:4539–4557

    Article  Google Scholar 

  • Tanaka K, Funakoshi Y, Hokamura T, Yamada F (2010) The role of paddy rice in recharging urban groundwater in the Shira River Basin. Paddy Water Environ 8:217–226

    Article  Google Scholar 

  • Terashima S, Ishihara S (1986) Copper, Lead, Zinc, Arsenic And Sulfur Of The Japanese Granitoids (3): Green Tuff Belt Of Northeast Japan And Outer Zone Of Southwest Japan. Bull Geol Surv Jpn 37(12):605–624

    Google Scholar 

  • Ure A, Berrow M (1982) The elemental constituents of soils. In: Bowen HJM (ed) Environmental Chemistry. Royal Society of Chemistry, London, pp 94–203

    Chapter  Google Scholar 

  • Walker FP, Schreiber ME, Rimstidt JD (2006) Kinetics of arsenopyrite oxidative dissolution by oxygen. Geochim Cosmochim Acta 70(7):1668–1676

    Article  Google Scholar 

  • Watanabe K (1978) Studies on the Aso pyroclastic flow deposits in the region to the west of Aso caldera, southwest Japan, I: geology of the Aso-4 pyroclastic flow deposits. Mem Fac Educ Kumamoto Univ Nat Sci 27:97–120

    Google Scholar 

  • Watanabe K (1979) Studies on the Aso pyroclastic flow deposits in the region to the west of Aso caldera, southwest Japan, II: petrology of the Aso-4 pyroclastic flow deposits. Mem Fac Educ Kumamoto Univ Nat Sci 28:75–112

    Google Scholar 

  • Welch AH, Westjohn DB, Helsel DR, Wanty RB (2000) Arsenic in ground water of the United States: occurrence and geochemistry. Ground Water 38:589–604

    Article  Google Scholar 

  • Wood WW (1981) Guidelines for collection and field analysis of ground-water samples for selected unstable constituents. US Geol. Surv. Techniques Water-Resour. Invest. Book 1 (Chapter D2)

  • Xie X, Wang Y, Su C, Liu H, Duan M, Xie Z (2008) Arsenic mobilization in shallow aquifers of Datong Basin: hydrochemical and mineralogical evidences. J Geochem Explor 98(3):107–115

    Article  Google Scholar 

  • Xie X, Ellis A, Wang Y, Xie Z, Duan M, Su C (2009) Geochemistry of redox-sensitive elements and sulfur isotopes in the high arsenic groundwater system of Datong Basin, China. Sci Total Environ 407(12):3823–3835

    Article  Google Scholar 

  • Zheng Y, Stute M, van Geen A, Gavrieli I, Dhar R, Simpson HJ, Schlosser P, Ahmed KM (2004) Redox control of arsenic mobilization in Bangladesh groundwater. Appl Geochem 19:201–214

    Article  Google Scholar 

Download references

Acknowledgments

This study was funded under the Core Research for Evolutional Science and Technology project (CREST) by the Japan Science and Technology Agency (JST) with additional from the Grant-in-Aid for young scientists (A) (no. 24681007). The authors wish to thank Dr. Kotaro Nakata of Central Research Institute of Electric Power Industry (CRIEPI) laboratory for rendering help in DOC analyses and Kumamoto city government office for supplying the sediment core samples. Special thanks are extended to Dr. Makoto Kagabu, Kumamoto University for his help in illustrating some maps and figures for this manuscript. We are grateful to Dr. Yang for his cordial help during sample collection. Finally, we are paying sincere thanks to two anonymous reviewers for their constructive and useful review comments to improve this manuscript.

Author information

Authors and Affiliations

  1. Graduate School of Science and Technology (GSST), Kumamoto University, 2-39-1 Kurokami, Kumamoto, 860-8555, Japan

    Shahadat Hossain, Kiyoshi Ide, Midori Matsunaga & Jun Shimada

  2. Priority Organization for Innovation and Excellence, Kumamoto University, 2-39-1 Kurokami, Kumamoto, 860-8555, Japan

    Takahiro Hosono

Authors
  1. Shahadat Hossain
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Takahiro Hosono
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Kiyoshi Ide
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Midori Matsunaga
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Jun Shimada
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Shahadat Hossain.

Electronic supplementary material

Below is the link to the electronic supplementary material.

Supplementary material 1 (DOCX 313 kb)

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Hossain, S., Hosono, T., Ide, K. et al. Redox processes and occurrence of arsenic in a volcanic aquifer system of Kumamoto Area, Japan. Environ Earth Sci 75, 740 (2016). https://doi.org/10.1007/s12665-016-5557-x

Download citation

  • Received:

  • Accepted:

  • Published:

  • DOI: https://doi.org/10.1007/s12665-016-5557-x

Keywords

Search

Navigation