Mechanism of Saponite Crystallization from a Rapidly Formed Amorphous Intermediate

Clays are crucial mineral phases in Earth’s weathering engine, but we do not know how they form in surface environments under (near-)ambient pressures and temperatures. Most synthesis routes, attempting to give insights into the plausible mechanisms, rely on hydrothermal conditions, yet many geological studies showed that clays may actually form at moderate temperatures (<100 °C) in most terrestrial settings. Here, we combined high-energy X-ray diffraction, infrared spectroscopy, and transmission electron microscopy to derive the mechanistic pathways of the low-temperature (25–95 °C) crystallization of a synthetic Mg-clay, saponite. Our results reveal that saponite crystallizes via a two stage process: (1) a rapid (several minutes) coprecipitation where ∼20% of the available magnesium becomes incorporated into an aluminosilicate network, followed by (2) a much slower crystallization mechanism (several hours to days) where the remaining magnesium becomes gradually incorporated into the growing saponite sheet structure.