Evidence for the accumulation of toxic metal(loid)s in agricultural soils impacted from long-term application of phosphate fertilizer.

Phosphate fertilizers may contain elevated concentrations of toxic metals and metalloids and therefore, their excessive application can result in the accumulation of both phosphorus (P) and metal(loid)s in agricultural soils. This study aims to investigate the occurrence, distribution, and potential plant-availability of metal(loid)s originating from phosphate fertilizer in a long-term experimental field at the Tidewater Research Station in North Carolina, where topsoil (10-20 cm deep) and subsoil (up to 150 cm deep) samples were collected from five plots with consistent and individually different application rates of P-fertilizer since 1966. We conducted systematic analyses of P and metal(loid)s in bulk soils, in the plant available fraction, and in four sequentially extracted soil fractions (exchangeable, reducible, oxidizable, and residual). The results show that P content in topsoils were directly associated with the rate of P-fertilizer application (ρ = 1, p < 0.05). Furthermore, P concentrations were highly correlated with concentrations of Cd, U, Cr, V, and As in the bulk topsoil (ρ > 0.58, p < 0.05), as well as the potential plant-available fraction (ρ > 0.67, p < 0.01), indicating the accumulation of the fertilizer-derived toxic metal(loid)s in the topsoil. Significant correlations (p < 0.001) of metal(loid)s concentrations between the bulk soil and the potential plant-available fraction raises the possibility that P-fertilizer application could increase the accumulation of toxic metal(loid)s in plants, which could increase human exposure. Results from sequential leaching experiments revealed that large portions of the trace elements, in particular Cd, occur in the soluble (exchangeable and reducing) fractions of topsoil with higher P-fertilizer input, whereas the levels of redox-sensitive elements (As, V, U, Cr) were higher in the reducible and oxidizable fractions of the soils. Overall, the data presented in this study demonstrate the effect of long-term P-fertilizer application on the occurrence and accumulation of a wide range of toxic metal(loid)s in agricultural topsoil.