Quantification of individual Rare Earth Elements from industrial sources in sewage sludge

Rare Earth Elements (REEs) are used in increasing amounts in technical applications and consumer products. However, to date, the contribution of industrial sources to the loads of individual REEs in wastewater streams have not been quantified. Here, we determine the REE contents in sludge collected from 63 wastewater treatment plants (WWTPs) across Switzerland. To quantify the industrial fraction of individual REEs in the sewage sludge, we develop two complementary approaches, based on REE ratios and REE pattern fitting. Unspecific (background) inputs, with REE patterns similar to the averaged REE pattern of soils collected across Switzerland, dominate the REE budget of most WWTPs. A few WWTPs receive significant REE inputs from specific industrial sources. Based on population equivalents of Switzerland, we estimate a total annual load of 4200 kg Cerium (Ce, 0.5 g Ce year^-1 capita^-1), with an industrial contribution of 2000 kg year^-1. The latter agrees with estimates of probabilistic mass flow models for engineered nanoscale CeO₂ particles discharged to the sewer network. About 7 kg year^-1 of Samarium (Sm,total for Switzerland: 184 kg year^-1 or 0.02 g Sm year^-1 capita^-1) and 3 kg year^-1 of Europium (Eu,total for Switzerland: 44 kg year^-1 or 0.005 g Eu year^-1 capita^-1) are assigned to industrial inputs from single WWTPs. Gadolinium (Gd) is used in the form of a stable complex as contrast agent in magnetic resonance imaging. Assuming 10% removal of Gd during wastewater treatment, we calculate an annual discharge of 90 kg of Gd from one individual WWTP to surface waters. WWTPs with exceptionally high industrial inputs of specific REEs warrant detailed investigations to identify the respective sources and to assess whether REE concentrations in effluents are elevated to the same degree.