Historical Hg accumulation (65 cal kyr BP) in upland lakes of the Southeastern Brazilian Amazonia: New evidence of the extent of geogenic and diagenetic control

The historical upland lake sediments in the Brazilian Amazon witnessed significant enrichment of total mercury (Hg). However, its spatio-temporal relationships between lakes and the main factors responsible for this enrichment are still poorly constrained. Given this, we geochemically investigated 12 radiometrically dated (extending back to 65 cal kyr BP) sediment cores from the Carajas plateau, Brazil. The Hg level in historical sediments presented a large temporal variability (from 1 to 3200 mu g/kg), with maximum accumulation peaks observed between 30 and 45 cal kyr BP in core R2, LB3, and R1. However, the lack of the Hg peak in other cores (LV2 and LTI3) during the same period despite being proximity and non-correlation of these Hg peaks with the onset of major volcanic events indicates that this source has little bearing. Hg enrichment is highly dependent on the type of sedimentary facies, with higher values were associated with detritic facies (MI) and detritic+organic facies (P/M). Principal component analysis shows that aluminosilicate minerals and organic matter are essential hosts of Hg in sediments. The positive correlation between Al, Ti, and Hg in detritic facies and their strong coherence with Hg/TOC in R1, R5, LSL, ST02, and LB3 cores indicate that Hg is primarily of lithogenic origin. This can be substantiated by the higher background threshold value of Hg (574 mu g/kg) in historical lake sediments compared to those in recent lake sediments (340 mu g/kg). However, the most pronounced Hg peak (3200 mu g/kg) in R2 around 45 cal kyr BP, which correlates positively with TOC, S, Se, As, and Mo indicates their diagenetic enrichment in organic-rich sediments under anoxic conditions. Thus, in addition to the lithogenic effect, it can be argued that diagenesis can play a significant role in prompting Hg enrichment in the Carajas lake sediments in Amazonia.