Fate of Arsenic and Trace Elements in Deep Aquifer

water of Bangladesh: Experimental Measurement

and Chemical Equilibrium Model

Mohammad Alauddin

Wagner College, NY, USA

WATER QUALITY ANALYSIS

SampleID

Conduc-tivity

µs

pH TDS

ppm

Fluoride

ppm

Chloride

ppm

Sulphate

ppm

Phosphate

ppm

B-1 444.00 7.60 222.00 0.25 57.66 2.37 < 0.005

B-2 375.00 7.30 182.00 0.39 22.50 1.36 < 0.005

B-3 309.00 7.40 150.00 0.37 30.50 2.57 0.007

B-4 384.00 7.35 178.00 0.41 19.94 1.06 0.04

B-5 320.00 7.60 164.00 0.47 19.82 1.09 0.13

B-6 846.00 7.45 415.00 0.14 133.90 10.90 < 0.005

B-7 280.00 8.05 145.00 0.31 13.42 0.08 < 0.005

B-8 752.00 7.40 361.00 0.14 113.50 4.66 0.05

B-9 429.00 7.45 205.00 0.15 20.74 1.25 <0.005

B-10 403.00 7.45 195.00 0.34 21.29 1.17 0.23

B-11 1,643.00 7.30 784.00 0.095 224.80 28.53 <0.005

B-12 444.00 7.45 212.00 0.30 37.41 1.53 0.23

B-13 535.00 7.45 254.00 0.28 48.90 3.98 <0.005

B-14 1,151.00 7.50 554.00 0.18 211.60 0.03 0.008

WATER QUALITY ANALYSISSample

IDNO2

-

ppm

NO3-

ppm

Br Fe

ppm

Mn

ppm

Total Hardness

ppm

As

ppb

B-1 < 0.005 < 0.005 0.22 0.63 0.09 39.30 < 2

B-2 < 0.005 0.04 0.02 0.71 0.40 60.12 < 2

B-3 < 0.005 0.01 0.10 2.94 0.11 30.46 3.52

B-4 < 0.005 <0.005 1.14 1.27 0.22 40.08 < 2

B-5 < 0.005 0.01 0.20 1.71 0.13 28.86 4.40

B-6 < 0.005 0.16 <0.005 1.15 0.46 57.71 < 2

B-7 < 0.005 0.02 0.10 0.45 0.13 20.84 < 2

B-8 < 0.005 0.14 1.21 1.11 0.82 76.15 < 2

B-9 < 0.005 0.06 <0.005 0.70 0.37 59.32 < 2

B-10 < 0.005 0.08 0.64 0.61 0.46 50.50 < 2

B-11 < 0.005 0.35 1.45 1.36 0.33 190.80 < 2

B-12 < 0.005 <0.005 0.24 6.18 0.66 50.50 3.46

B-13 < 0.005 0.03 0.74 1.25 0.57 69.74 < 2

B-14 < 0.005 < 0.005 1.09 0.76 0.13 81.76 < 2

Deep Tube Well Water Samples

Sample ID Description Ba(ppb) B (ppb) Pb (ppb) Cr (ppb) Mn (ppb) Co (ppb) Cu (ppb) Cd (ppb)

1 Vill: Kulia 158 131 <1.00 1.51 23.6 4.66 106 <1.002 Shahid Islam 264 137 <1.00 <0.10 <0.50 5.09 <0.50 <1.003 Bashir Zaman 154 147 <1.00 <0.10 65.6 5.32 <0.50 <1.004 Bazlur Rahman 147 145 <1.00 <0.10 <0.50 7.56 <0.50 <1.005 Sahabuddin 176 136 <1.00 <0.10 <0.50 6.66 <0.50 <1.006 Abdul Ohab 184 141 <1.00 <0.10 <0.50 6.94 <0.50 <1.007 Hafizur Rahman 183 146 <1.00 <0.10 <0.50 6.76 0.68 <1.008 Zikorgacha 102 139 <1.00 20.2 101 8.28 <0.50 <1.009 Kamal Hossain 123 159 <1.00 4.20 36.7 10.2 <0.50 <1.0010 Mohar Ali 83.0 149 <1.00 <0.10 <0.50 9.33 <0.50 <1.0011 GM Zahangir 117 156 <1.00 0.68 <0.50 9.72 33.0 <1.0012 Mafizur Rahman 146 151 <1.00 <0.10 <0.50 10.1 <0.50 <1.0013 Karim Ali 164 154 <1.00 0.87 1.24 11.4 <0.50 <1.0014 Tapas Kumar 132 152 <1.00 <0.10 53.8 12.9 <0.50 <1.0015 MA Aziz 136 148 <1.00 0.21 57.6 12.2 <0.50 <1.00

Sample ID pH Cond.(uS)Turbidity(NTU)Hardness(ppm) Iron(ppm) As(ppb)

Mohar Ali 5.75 885 0.20 155 0.74 48.6

Bashirujjaman 6.95 920 0.40 168 0.42 <2.0

Dr. Hafijur Rahman 6.70 1309 1.24 189 0.65 <2.0

Karim Ali 6.75 1504 0.60 135 1.06 4.4

G.M. Jahangir 6.85 1493 0.50 62.5 0.20 <2.0

Abdul Wahab Member 6.65 1438 0.36 152 1.03 2.6

Md. Shahabuddin 6.45 1082 0.24 231 0.11 <2.0

Kulia 6.65 951 0.34 204 0.50 <2.0

Kamal Hossain 7.05 1796 0.36 45.7 0.17 <2.0

M.A. Aziz 6.95 625 0.36 83.3 0.20 2.4

Zhikorgacha 3.15 1283 0.41 135 1.31 <2.0

Md. Shahidul Islam 6.65 849 0.86 177 0.93 <2.0

Bazlur Rahman 6.55 804 1.09 130 1.63 62.4

Taposh Kumar Ghosh 6.75 1557 2.90 223 1.31 2.6

Md. Hafijur Rahman 7.15 780 0.23 78.5 0.14 <2.0

Sample ID Fluoride(ppm) Chloride(ppm) Nitrite(ppm) Nitrate(ppm) Bromide(ppm)Sulphate(ppm) Phosphate(ppm)

Mohar Ali 0.10 251 0.040 3.25 0.090 0.13 0.070

Bashirujjaman 0.11 41.3 1.27 1.84 0.13 0.03 0.020

Dr. Hafijur Rahman 0.13 278 <.005 0.007 0.79 0.04 0.008

Karim Ali 0.11 325 <0.005 3.25 0.99 0.01 <0.005

G.M. Jahangir 0.15 259 <0.005 3.93 0.68 0.3 0.22

Abdul Wahab Member 0.21 71.9 <.005 2.46 0.21 0.08 0.10

Md. Shahabuddin 0.090 54.9 <.005 12.3 0.13 12.3 0.010

Kulia 0.10 50.2 0.18 98.9 0.14 22.7 0.060

Kamal Hossain 0.23 361 1.02 4.05 1.19 0.009 0.33

M.A. Aziz 0.070 14.9 1.34 0.020 0.32 0.09 0.020

Zhikorgacha 0.17 23.2 <0.005 5.47 1.04 1.79 0.12

Md. Shahidul Islam 0.080 17.8 0.010 0.98 0.06 0.03 <0.005

Bazlur Rahman 0.070 9.72 0.080 4.78 <.005 0.08 0.070

Taposh Kumar Ghosh 0.070 399 <0.005 0.020 1.24 0.02 0.010

Md. Hafijur Rahman 0.070 70.3 1.21 0.050 0.17 0.17 0.010

Deep well water GOOD FIT Charge balance = 2.9%Calculated ionic strength = 0.0114 p(CO2) = 0.0206 atmSpecies Concentration (M) Activity Log activityAsO3-3 2.8218E-24 1.0546E-24 -23.977AsO4-3 7.9485E-14 2.9706E-14 -13.527Ba+2 6.035E-07 3.8968E-07 -6.409BaCO3 (aq) 9.2099E-13 9.2341E-13 -12.035BaH2BO3+ 6.0587E-14 5.431E-14 -13.265BaHCO3+ 7.2759E-10 6.5222E-10 -9.186BaNO3+ 1.0157E-10 9.1046E-11 -10.041BaOH+ 1.0743E-14 9.6299E-15 -14.016HSO4- 4.7631E-12 4.2697E-12 -11.37NO2-1 8.6946E-07 7.7939E-07 -6.108NO3-1 0.000052005 0.000046618 -4.331OH- 6.3155E-09 5.6612E-09 -8.247PO4-3 1.6816E-14 6.2846E-15 -14.202SO4-2 3.8051E-08 2.4569E-08 -7.61H2AsO4- 3.0223E-07 2.7092E-07 -6.567H2BO3- 5.0312E-09 4.51E-09 -8.346H2CO3* (aq) 0.00069911 0.00070095 -3.154H2PO4- 8.2941E-07 7.4349E-07 -6.129H3AsO3 3.2806E-07 3.2892E-07 -6.483H3AsO4 8.3505E-11 8.3724E-11 -10.077

SPECIES DISTRIBUTION WHEN ALL IRON PPT OUT AND ACT AS SURFACE COMPLEXING AGENT

Hydrous ferric oxide = 10mg/L, Surface area = 300 m^2/gCalculated surface potential = 96 mV Strong site = 0.1 mmol/kgCharge balance = 3% good Weak site = 1.0 mmol/kgSpecies Concentration Activity Log activity>FeCO3- (1) 0.00020221 0.00020221 -3.694>FeCO3H (1) 0.00032192 0.00032192 -3.492>FeH2AsO3 (1) 2.9515E-07 2.9515E-07 -6.53>FeH2AsO4 (1) 1.0852E-10 1.0852E-10 -9.964>FeH2BO3 (1) 1.4935E-08 1.4935E-08 -7.826>FeH2PO4 (1) 1.8058E-08 1.8058E-08 -7.743>FeHAsO4- (1) 4.203E-09 4.203E-09 -8.376>FehCO3- (1) 0.000019593 0.000019593 -4.708>FehCO3H (1) 0.000031193 0.000031193 -4.506>FehH2AsO3 (1) 2.8599E-08 2.8599E-08 -7.544>FehH2AsO4 (1) 1.0515E-11 1.0515E-11 -10.978>FehH2BO3 (1) 1.4471E-09 1.4471E-09 -8.839>FehH2PO4 (1) 1.7498E-09 1.7498E-09 -8.757>FehHAsO4- (1) 4.0725E-10 4.0725E-10 -9.39

All Fe(III) all preciptated J1 Deep w ellequal site density for strong and w eakCalc surface pot 70 mV 3% charge balance

Component Total dissolved % dissolved Total sorbed % sorbed Total precipitated% precipitatedAsO4-3 3.5045E-09 1.068 3.2468E-07 98.932 0 0Ba+2 6.0409E-07 99.959 2.4652E-10 0.041 0 0Ca+2 0.0038668 99.987 5.103E-07 0.013 0 0Cl-1 0.0070516 100 0 0 0 0CO3-2 0.00089069 98.871 0.000010169 1.129 0 0Fe+3 1.7906E-06 100 0 0 0 0H+1 0.0015803 98.562 0.000023065 1.438 0 0H3AsO3 2.0712E-07 63.114 1.2104E-07 36.886 0 0H3BO3 0.000013779 99.999 1.3059E-10 0.001 0 0NO2-1 8.6946E-07 100 0 0 0 0NO3-1 0.000052415 100 0 0 0 0PO4-3 2.6421E-08 2.788 9.2123E-07 97.212 0 0SO4-2 5.1746E-08 99.415 3.0438E-10 0.585 0 0

EQUILIBRATED MASS DISTRIBUTION OF COMPONENTS (MAIN SPEICES)Fe surface complex is considered at the input pHpH change can signifcantly alter distribution

ComponentTotal dissolved% dissolvedTotal sorbed% sorbed Total precipitated% precipitatedAsO4-3 4.019E-12 0.001 3.282E-07 99.999 0 0 ALL SORBED ON FeOOHBa+2 6.028E-07 99.752 1.497E-09 0.248 0 0Ca+2 0.0038642 99.919 3.114E-06 0.081 0 0Cl-1 0.0070516 100 0 0 0 0CO3-2 0.000326 36.182 0.0005749 63.818 0 0Fe+3 1.791E-06 100 0 0 0 0H+1 0.0005773 33.446 0.0011487 66.554 0 0H3AsO3 4.411E-09 1.344 3.238E-07 98.656 0 0 SIMILARH3BO3 1.376E-05 99.881 1.638E-08 0.119 0 0NO2-1 8.695E-07 100 0 0 0 0NO3-1 5.242E-05 100 0 0 0 0PO4-3 9.554E-11 0.01 9.476E-07 99.99 0 0SO4-2 1.63E-08 31.317 3.575E-08 68.683 0 0

ADSORPTION AND SURFECE COMPLEXATION IS PRIMARY MODE OF SPECIES IMMOBILIZATION

Concentration Activ ity Log activ ity

>FeCO3- (1) 1.2801E-06 1.2801E-06 -5.893

>FeCO3H (1) 3.9541E-06 3.9541E-06 -5.403

>FeH2AsO3 (1) 6.2303E-08 6.2303E-08 -7.205

>FeH2AsO4 (1) 4.2527E-10 4.2527E-10 -9.371

>FeH2BO3 (1) 6.7215E-11 6.7215E-11 -10.173

>FeH2PO4 (1) 2.2446E-08 2.2446E-08 -7.649

>FeHAsO4- (1) 8.4888E-09 8.4888E-09 -8.071

>FehCO3- (1) 1.2069E-06 1.2069E-06 -5.918

>FehCO3H (1) 3.7281E-06 3.7281E-06 -5.429

>FehH2AsO3 (1) 5.8742E-08 5.8742E-08 -7.231

>FehH2AsO4 (1) 4.0096E-10 4.0096E-10 -9.397

>FehH2BO3 (1) 6.3373E-11 6.3373E-11 -10.198

>FehH2PO4 (1) 2.1163E-08 2.1163E-08 -7.674

>FehHAsO4- (1) 8.0037E-09 8.0037E-09 -8.097

>FehHPO4- (1) 3.3555E-07 3.3555E-07 -6.474

>FehO- (1) 1.6287E-08 1.6287E-08 -7.788

>FehOH2+ (1) 0.000001704 0.000001704 -5.769

J1 more realistic

Assume oxic condition and all Fe(II) to Fe(III)Without surface complexation or Adsorption

Mineral log IAP Sat. IndexStoichiometryANHYDRITE -10.21 -5.853 1 Ca+2 1 SO4-2ARAGONITE -10.94 -2.603 1 Ca+2 1 CO3-2ARSENOLITE -25.93 -23.17 4 H3AsO3 -6 H2OAs2O5 -27.05 -33.76 2 AsO4-3 -3 H2OBa(OH)2:8H2O 5.09 -19.3 1 Ba+2 10 H2O -2 H+1Ba3(AsO4)2 -46.28 3.818 3 Ba+2 2 AsO4-3BaHPO4 -26.36 -6.586 1 Ba+2 1 H+1 1 PO4-3BARITE -14.02 -4.039 1 Ba+2 1 SO4-2Ca3(AsO4)2:4H2O -34.87 -15.97 3 Ca+2 2 AsO4-3 4 H2OCa3(PO4)2 (beta) -36.21 -7.293 3 Ca+2 2 PO4-3Ca4H(PO4)3:3H2O -58.77 -11.69 4 Ca+2 1 H+1 3 PO4-3 3 H2OFERRIHYDRITE 4.547 1.356 1 Fe+3 3 H2O -3 H+1GOETHITE 4.547 4.056 1 Fe+3 2 H2O -3 H+1GYPSUM -10.21 -5.603 1 Ca+2 1 SO4-2 2 H2OHEMATITE 9.094 10.512 2 Fe+3 3 H2O -6 H+1H-JAROSITE -24.58 -12.48 -5 H+1 3 Fe+3 2 SO4-2 7 H2OHYDROXYLAPATITE -49.87 -5.539 5 Ca+2 3 PO4-3 1 H2O -1 H+1LEPIDOCROCITE 4.547 3.176 -3 H+1 1 Fe+3 2 H2OLIME 8.896 -23.8 -2 H+1 1 Ca+2 1 H2OMAGHEMITE 9.094 2.708 -6 H+1 2 Fe+3 3 H2O

Mineral log IAP Sat. Index StoichiometryANHYDRITE -10.213 -5.853 1 Ca+2 1 SO4-2ARAGONITE -10.939 -2.603 1 Ca+2 1 CO3-2ARSENOLITE -25.931 -23.171 4 H3AsO3 -6 H2OAs2O5 -27.054 -33.76 2 AsO4-3 -3 H2OBa(OH)2:8H2O 5.09 -19.304 1 Ba+2 10 H2O -2 H+1Ba3(AsO4)2 -46.282 3.818 3 Ba+2 2 AsO4-3 pptedBaHPO4 -26.361 -6.586 1 Ba+2 1 H+1 1 PO4-3BARITE -14.019 -4.039 1 Ba+2 1 SO4-2Ca3(AsO4)2:4H2O -34.865 -15.965 3 Ca+2 2 AsO4-3 4 H2OCa3(PO4)2 (beta) -36.214 -7.294 3 Ca+2 2 PO4-3Ca4H(PO4)3:3H2O -58.77 -11.69 4 Ca+2 1 H+1 3 PO4-3 3 H2OCaCO3xH2O -10.939 -3.795 1 Ca+2 1 CO3-2 1 H2OCaHPO4 -22.555 -3.28 1 Ca+2 1 H+1 1 PO4-3CaHPO4:2H2O -22.555 -3.56 1 Ca+2 1 H+1 1 PO4-3 2 H2OCALCITE -10.939 -2.459 1 Ca+2 1 CO3-2CLAUDETITE -25.931 -22.866 4 H3AsO3 -6 H2OFe(OH)2 5.562 -8.002 1 Fe+2 2 H2O -2 H+1GYPSUM -10.213 -5.603 1 Ca+2 1 SO4-2 2 H2OHYDROXYLAPATITE -49.873 -5.54 5 Ca+2 3 PO4-3 1 H2O -1 H+1LIME 8.896 -23.803 -2 H+1 1 Ca+2 1 H2O

Conclusions

*Under anoxic condition Ba helps precipitation of As*Fate and speciation of As and other component are linked to formation of HFO.*Adsorption and surface complexation are responsible for species immobilization*Arsenite,Arsenate,Phosphate are believed to be fully adsorbed on the HFO.*Deep aquifer water seems to be a safe drinking water option at least for a short term

Acknowledgements

The work was partially supported by a grant from Wagner College, New York, USA

The work was also supported by a grant from The National Science Foundation (USA)

Margaret Fiasconaro

Sarah Alauddin

Wagner College, NY, USA

Maya Bhattacharjee

Shamima Sultana

Exonics Technology Center, Dhaka

Abul Hussam

George Mason University, USA

Mohammad Zakariya

BRAC, Dhaka