Interactions between viruses and goethite during saturated flow: Effects of solution pH, carbonate, and phosphate

Metal oxides have great potential for controlling the fate and transport of viruses in the subsurface and water-treatment systems. The processes, however, are subject to solution chemistry. In this study, a number of column experiments were conducted to examine the effects of solution pH and anions (carbonate and phosphate) on attachment, transport, and inactivation of two bacteriophages (ϕX174 and MS-2) in goethite-coated sand medium. Removal of both viruses on goethite-coated sand increased as solution pH decreased from 9.3 to 7.5, due mostly to virus inactivation. MS-2, a relatively hydrophobic virus with a lower isoelectric point (3.9), was more sensitive to the change of solution pH than ϕX174, a relatively hydrophilic virus with a higher isoelectric point (6.6), in terms of their attachment and inactivation on goethite. About 90% of the MS-2 particles removed by goethite (accounting for 81% of the total input) were inactivated at pH 7.5, whereas all of the removed MS-2 particles (accounting for 10% of the total input) still remained infectious at pH 9.3. In comparison, ~ 74% of the goethite-bound ϕX174 particles (accounting for 95% of the total input) lost their infectivity at pH 7.5, in contrast to a complete recovery at pH 9.3 (accounting for 65% of the total input) when the columns were eluted using a beef extract solution (pH 9.5). Presence of phosphate (20 mM H2PO4−) in input solution reduced virus attachment and appeared to protect the viruses from being inactivated during transport; this effect was more significant on MS-2 than on ϕX174. Specifically, ~ 29% of the ϕX174 particles and ~ 49% of MS-2 particles injected into the column were removed during transport. Mass recovery data showed that no ϕX174 was inactivated in the presence of phosphate, whereas about 38% of the MS-2 particles attached on goethite lost their infectivity. Conversely, presence of carbonate on goethite increased virus attachment and inactivation due to contribution of additional attachment sites from protonated surface groups of the carbonate ions that were adsorbed on goethite. About 70% of the total input viruses (both ϕX174 and MS-2) were removed during transport, of which 35% ϕX174 and 85% MS-2 were eventually inactivated.