The production of biogenic silica has dominated the marine silica cycle since early Paleozoic time, drawing down the concentration of dissolved silica in modern seawater to a few parts per million (ppm). Prior to the biological innovation of the first silica biomineralizing organisms in late Proterozoic time, inputs of silica into Precambrian seawater were balanced by strictly chemical silica and silicate precipitation processes, although the mechanics of this abiotic marine silica cycle remain poorly understood. Cherty sedimentary rocks are abundant in Archean sequences, and many previous authors have suggested that primary precipitation of amorphous silica could have occurred in Archean seawater. The recent discovery that many pure chert layers in early Archean rocks formed as sedimentary beds of sand-sized, subspherical silica granules has provided direct evidence for primary silica deposition. Here, we provide further sedimentological and geochemical analyses of early Archean silica granules in order to gain a better understanding of the mechanisms of granule formation. Silica granules are common components of sedimentary cherts from a variety of depositional settings and water depths. The abundance and widespread distribution of silica granules in Archean rocks suggest that they represented a significant primary silica depositional mode and that most formed by precipitation in the upper part of the water column. The regular occurrence of silica granules as centimeter-scale layers within banded chert alternating with layers of black or ferruginous chert containing few granules indicates episodic granule sedimentation. Contrasting silicon isotopic compositions of granules from different depositional environments indicate that isotopic signatures were modified during early diagenesis. Looking to modern siliceous sinters for insight into silica precipitation, we suggest that silica granules may have formed via multiple stages of aggregation of silica nanospheres and microspheres. Consistent with this hypothesis, Archean ocean chemistry would have favored particle aggregation over gelling. Granule formation would have been most favorable under conditions promoting rapid silica polymerization, including high salinity and/or high concentrations of dissolved silica. Our observations suggest that granule sedimentation was often episodic, suggesting that granule formation may have also been episodic, perhaps linked to variations in these key parameters.

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