Characterization of serpentinization in olivine-orthopyroxene-H₂O system revealed by thermogravimetric and multivariate statistical analyses

Thermogravimetric (TG) analyses were used to characterize the products and quantify the extent of serpentinization as a stepwise weight loss during heating (TG loss) or its derivative (DTG). Multivariate analyses are powerful tools for extracting information from complicated spectrum data; however, no studies have applied them to characterize serpentinites. In this study, hydrothermal experiments of olivine-H2O, olivine-orthopyroxene-H2O and orthopyroxene-H2O were conducted at 250-400 degrees C and under vapor-saturated pressure. The product minerals observed were serpentine+brucite+magnetite in the olivine-H2O experiments and serpentine +/- talc in the orthoyroxene-H2O and olivine-orthopyroxene-H2O experiments. These results are consistent with those of previous studies; however, the positions and width of DTG peaks for individual minerals were varied depending on the experimental conditions. To extract systematics from the TG spectra, non-negative matrix factorization (NMF), an unsupervised machine learning technique, was applied to the DTG spectra of the experimental products. NMF revealed that the DTG profiles were explained by a linear combination of six basis spectra, which corresponded to the characteristic products, including three types of serpentine minerals (low-, medium-, and high-T), two types of brucite (low-and high-T), two type of talc (talc+serpentine mixture, well-crystallized talc) with different crystallinity, and noise during the TG measurement. Systematic changes in the factor loading revealed that, in the olivine-H2O systems, the products changed from medium-T serpentine+low-T brucite to high-T serpentine+high-T brucite as serpentinization progressed. In the olivine-orthopyroxene system, low-T serpentine or poorly crystallized talc+serpentine mixture was initially formed, followed by the formation of well-crystallized talc, resulting in dehydration. Applying NMF to DTG showed the mineralogical differences between olivine and orthopyroxene systems and increases of the crystallinity during the progress of serpentinization, suggesting its potential for characterizing various serpentinites within oceanic lithospheres that suffer from several stages of alteration and weathering at different temperatures.