In this paper, a numerical model to simulate the hydraulic conductivity reduction observed during long-term laboratory column tests is proposed. The column tests are carried out to study dissolved heavy metals removal by using granular zero valent iron (ZVI). The proposed model is also used to analyse the main causes of hydraulic conductivity reduction observed during laboratory column tests. Expansive iron corrosion, precipitation of reaction products, and gas formation are the processes considered in the proposed model. Numerical simulation results show that to reproduce hydraulic behaviour of the experimental systems, the change of pores geometry due to expansive iron corrosion and precipitation of reaction products, which determines a possible stoppage of gas bubbles, should be considered. Furthermore, model results show that only a small percentage of the iron available is corroded during the tests (from 0.4% to 1.9%). According to the model, the average diameter of gas bubbles that better fit the experimental results varies between 0.16 and 0.19 mm. While assuming gas absence (or its possible escape), higher values of iron corrosion rate should be considered to fit the experimental results.

Metallic iron (Fe(0)) is currently used in subsurface and above-ground water filtration systems on a pragmatic basis. Recent theoretical studies have indicated that, to be sustainable, such systems should not contain more than 60% Fe(0) (vol/vol). The prediction was already validated in a Fe(0)/sand system using methylene blue as an operational tracer. The present work is the first attempt to experimentally verify the new concept using pumice particles. A well-characterized pumice sample is used as operational supporting material and is mixed with 200 g of a granular Fe(0), in volumetric proportions, varying from 0 to 100%. The resulting column systems are characterized (i) by the time dependent evolution of their hydraulic conductivity and (ii) for their efficiency for the removal of Cu(II), Ni(II), and Zn(II) from a three-contaminants-solution (about 0.3 mM of each metal). Test results showed a clear sustainability of the long term hydraulic conductivity with decreasing Fe(0)/pumice ratio. In fact, the pure Fe(0) system clogged after 17 days, while the 25% Fe(0) system could operate for 36 days. The experimental data confirmed the view that well-designed Fe(0) PRBs may be successful at removing both reducible and non-reducible metal species.

Running Title: Admixing pumice and sand to reactive Fe 0 sustains long-term metal removal. Acronym List PRB Permeable Reactive Barrier

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