Nitrate removal by a permeable reactive barrier of Fe⁰: A model-based evaluation

Abstract

Permeable reactive barrier (PRB) filled with zero valent iron (ZVI, Fe⁰) can be an effective option to remove nitrate from contaminated groundwater. The long-term performance of such PRBs, however, might be compromised by the problem of declining reactivity and permeability, which could cause a decrease in the nitrate removal efficiency. In this study we explored suitable model formulations that allow for a process-based quantification of the passivation effect on denitrification rates and tested the model for a 40 years long operation scenario. The conceptual model underlying our selected formulation assumes the declining reactivity of the ZVI material through the progressing passivation caused by the precipitation of secondary minerals and the successive depletion of the ZVI material. Two model scenarios, i.e., the base model scenario which neglects the explicit consideration of the passivation effect and one performed with the model in which the impact of the passivation effect on denitrification was considered, were compared. The modeling results illustrate that nitrate removal in the model of considered passivation started to be incomplete after 10 years, and the effluent nitrate concentration of PRB rose up to 86% of the injected water concentration after 40 years, in contrast to the base scenario, corresponding well with the field observations of successively declining nitrate removal efficiencies. The model results also showed that the porosity of the PRB increased in both models. In order to improve and recover the reactivity of ZVI, pyrite was added to the PRB, resulting in completely nitrate removal and lower consumption of ZVI.

Keywords

groundwater / permeable reactive barrier / zero valent iron / PHT3D / denitrification

References

[1] China Geological Survey, 2012. Handbook of Hydrogeology (2nd Version). Geological Publishing House, Beijing

[2] Choe S., Chang Y. Y., Hwang K. Y., . Kinetics of Reductive Denitrification by Nanoscale Zero-Valent Iron. Chemosphere, 2000, 41(8): 1307-1311.

[3] Choe S., Liljestrand H. M., Khim J. Nitrate Reduction by Zero-Valent Iron under Different pH Regimes. Applied Geochemistry, 2004, 19(3): 335-342.

[4] Clement T. P. A Modular Computer Code for Simulating Reactive Multi-Species Transport in 3-Dimensional Groundwater Aquifers, 1997, Washington: Pacific Northwest National Laboratory

[5] Cohen E. L., Patterson B. M., McKinley A. J., . Zero Valent Iron Remediation of a Mixed Brominated Ethene Contaminated Groundwater. Journal of Contaminant Hydrology, 2009, 103(3/4): 109-118.

[6] Liou Y. H., Lo S. L., Lin C. J., . Methods for Accelerating Nitrate Reduction Using Zero-Valent Iron at Near-Neutral pH: Effects of H2-Reducing Pretreatment and Copper Deposition. Environmental Science & Technology, 2005, 39(24): 9643-9648.

[7] Henderson A. D., Demond A. H. Long-Term Performance of Zero-Valent Iron Permeable Reactive Barriers: A Critical Review. Environmental Engineering Science, 2007, 24(4): 401-423.

[8] Huang Y. H., Zhang T. C. Kinetics of Nitrate Reduction by Iron at near Neutral pH. Journal of Environmental Engineering, 2002, 128(7): 604-611.

[9] Huang Y. Y., Liu D. D., Li G. R. Adsorption Kinetics of As (?) from Groundwater by Nanoscale Zero-Valent Iron. Earth Science–Journal of China University of Geosciences, 2012, 37(2): 294-300.

[10] Jeen S. W., Amos R. T., Blowes D. W. Modeling Gas Formation and Mineral Precipitation in a Granular Iron Column. Environmental Science & Technology, 2012, 46(12): 6742-6749.

[11] Jeen S. W., Gillham R. W., Przepiora A. Predictions of Long-Term Performance of Granular Iron Permeable Reactive Barriers: Field-Scale Evaluation. Journal of Contaminant Hydrology, 2011, 123(1/2): 50-64.

[12] Jeen S., Gillham R. W., Blowes D. W. Effects of Carbonate Precipitates on Long-Term Performance of Granular Iron for Reductive Dechlorination of TCE. Environmental Science & Technology, 2006, 40(20): 6432-6437.

[13] Jeen S., Mayer K. U., Gillham R. W., . Reactive Transport Modeling of Trichloroethene Treatment with Declining Reactivity of Iron. Environmental Science & Technology, 2007, 41(4): 1432-1438.

[14] Jin S. O., Jeen S. W., Gillham R., . Effects of Initial Iron Corrosion Rate on Long-Term Performance of Iron Permeable Reactive Barriers: Column Experiments and Numerical Simulation. Journal of Contaminant Hydrology, 2009, 103(3/4): 145-156.

[15] Johnson R. L., Thoms R. B., O’Brien Johnson R., . Mineral Precipitation Upgradient from a Zero-Valent Iron Permeable Reactive Barrier. Ground Water Monitoring & Remediation, 2008, 28(3): 56-64.

[16] Kamolpornwijit W., Liang L., West O. R., . Preferential Flow Path Development and Its Influence on Long-Term PRB Performance: Column Study. Journal of Contaminant Hydrology, 2003, 66(3–4): 161-178.

[17] Liang L. Y., Moline G. R., Kamolpornwijit W., . Influence of Hydrogeochemical Processes on Zero-Valent Iron Reactive Barrier Performance: A Field Investigation. Journal of Contaminant Hydrology, 2005, 78(4): 291-312.

[18] Mayer K. U., Blowes D. W., Frind E. O. Reactive Transport Modeling of an in Situ Reactive Barrier for the Treatment of Hexavalent Chromium and Trichloroethylene in Groundwater. Water Resources Research, 2001, 37(12): 3091-3103.

[19] Nyirenda T. M., Zhou J. W., Xie L. N., . Determination of Carbonate Minerals Responsible for Alkaline Mine Drainage at Xikuangshan Antimony Mine, China: Using Thermodynamic Chemical Equilibrium Model. Journal of Earth Science, 2015, 26(5): 755-762.

[20] Parkhurst D. L., Appelo C. A. J. User’s Guide to PHREEQC (Version 2)-A Computer Program for Speciation, Batch-Reaction, One-Dimensional Transport, and Inverse Geochemical Calculations, 1999.

[21] Prommer H., Aziz L. H. B., o N., . Modelling of Geochemical and Isotopic Changes in a Column Experiment for Degradation of TCE by Zero-Valent Iron. Journal of Contaminant Hydrology, 2008, 97(1/2): 13-26.

[22] Robertson W. D., Cherry J. A. In Situ Denitrification of Septic-System Nitrate Using Reactive Porous Media Barriers: Field Trials. Ground Water, 1995, 33(1): 99-111.

[23] Robertson W. D., Ptacek C. J., Brown S. J. Geochemical and Hydrogeological Impacts of a Wood Particle Barrier Treating Nitrate and Perchlorate in Ground Water. Ground Water Monitoring & Remediation, 2007, 27(2): 85-95.

[24] Robertson W. D., Blowes D. W., Ptacek C. J., . Long-Term Performance of in Situ Reactive Barriers for Nitrate Remediation. Ground Water, 2000, 38(5): 689-695.

[25] Rodríguez-Maroto J. M., García-Herruzo F., García-Rubio A., . Kinetics of the Chemical Reduction of Nitrate by Zero-Valent Iron. Chemosphere, 2009, 74(6): 804-809.

[26] RTDF, Remediation Technologies Development Forum. 2001. Permeable Reactive Barrier Installation Profiles. [2017-03-16]. http://www.rtdf.org/public/permbarr/prbsumms/default.cfm.

[27] Till B. A., Weathers L. J., Alvarez P. J. J. Fe(0)-Supported Autotrophic Denitrification. Environmental Science & Technology, 1998, 32(5): 634-639.

[28] Wilkin R. T., Puls R. W., Sewell G. W. Long-Term Performance of Permeable Reactive Barriers Using Zero-Valent Iron: Geochemical and Microbiological Effects. Ground Water, 2003, 41(4): 493-503.

[29] Thiruvenkatachari R., Vigneswaran S., Naidu R. Permeable Reactive Barrier for Groundwater Remediation. Journal of Industrial and Engineering Chemistry, 2008, 14(2): 145-156.

[30] Vogan J. L., Focht R. M., Clark D. K., . Performance Evaluation of a Permeable Reactive Barrier for Remediation of Dissolved Chlorinated Solvents in Groundwater. Journal of Hazardous Materials, 1999, 68(1/2): 97-108.

[31] Zhang J. H., Hao Z. W., Zhang Z., . Kinetics of Nitrate Reductive Denitrification by Nanoscale Zero-Valent Iron. Process Safety and Environmental Protection, 2010, 88(6): 439-445.

[32] Zhang Z., Hao Z. W., Yang Y. P., . Reductive Denitrification Kinetics of Nitrite by Zero-Valent Iron. Desalination, 2010, 257(1/2/3): 158-162.

[33] Zhang Y. S., Gillham R. W. Effects of Gas Generation and Precipitates on Performance of Fe0 PRBs. Ground Water, 2005, 43(1): 113-121.

[34] Zheng, C., Wang, P. P., 1999. MT3DMS: A Modular Three-Dimensional Multispecies Transport Model for Simulation of Advection, Dispersion, and Chemical Reactions of Contaminants in Groundwater Systems, Documentation and User’s Guide. Contract Report SERDP-99-1, U.S. Vicksburg, Army Engineer Research and Development Center, Mississippi

[35] Schipper L., Vojvodic-Vukovic M. Nitrate Removal from Groundwater Using a Denitrification Wall Amended with Sawdust: Field Trial. Journal of Environment Quality, 1998, 27 3 664

[36] Mackenzie P. D., Horney D. P., Sivavec T. M. Mineral Precipitation and Porosity Losses in Granular Iron Columns. Journal of Hazardous Materials, 1999, 68(1/2): 1-17.

[37] Alowitz M. J., Scherer M. M. Kinetics of Nitrate, Nitrite, and Cr (VI) Reduction by Iron Metal. Environmental Science & Technology, 2002, 36(3): 299-306.

[38] Li L., Benson C. H., Lawson E. M. Impact of Mineral Fouling on Hydraulic Behavior of Permeable Reactive Barriers. Ground Water, 2005, 43(4): 582-596.

[39] Chen Y. M., Li C. W., Chen S. S. Fluidized Zero Valent Iron Bed Reactor for Nitrate Removal. Chemosphere, 2005, 59(6): 753-759.

[40] Robertson W. D., Vogan J. L., Lombardo P. S. Nitrate Removal Rates in a 15-Year-Old Permeable Reactive Barrier Treating Septic System Nitrate. Ground Water Monitoring & Remediation, 2008, 28(3): 65-72.

[41] Hwang Y. H., Kim D. G., Shin H. S. Mechanism Study of Nitrate Reduction by Nano Zero Valent Iron. Journal of Hazardous Materials, 2011, 185(2–3): 1513-1521.