The lithium-rich brines of the Salar de Olaroz in the Central Andes of NW Argentina are considered to be of great economic and strategic interest. This study focused on the fluid source(s) and geochemical processes governing the chemical and isotopic characteristics of the surficial waters of Olaroz (residual brines, ephemeral lakes, rivers and tributary streams), aiming to define the mechanisms leading to such a huge Li reservoir. The chemistry of the Rosario River, which is one of the main sources of recharge of the Salar de Olaroz, is mostly controlled by fluid inputs from hydrothermal systems located north of the salar (in the volcanic areas of Rosario de Coyaguayma, Pairique, and Cono Panizo). The hydrothermal fluids are characterized by relatively high Li concentrations, as they interact with Li-rich rocks pertaining to Miocene -Pliocene volcanic formations, Ordovician sedimentary deposits, and, possibly, pre-Ordovician crystalline basement. In the salar, the hyperarid climate regulates the relative proportion between supplied waters and evaporation, inducing deposition/dissolution of salts, which controls the concentrations of main ions in brines and ephemeral lakes. Hence, the peculiar combination of a Lirich primary source, the hydrothermal scavenging by geothermal fluids that feed the Rosario River, and secondary concentration processes affecting the surficial water within the salar leads to the formation of the huge Li reservoir characterizing this area.
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