Evolution of organo-clay composites with respect to thermal maturity in type II organic-rich source rocks

Among the proposed pathways of sequestration and progressive transformation of organic matter (OM) during burial, the sorptive protection mechanism explains the strong relationship between total organic carbon (TOC) and mineral surface area (MSA) noted in numerous black shales around the globe. The complete mechanistic framework of preservation and evolution of OM in organo-mineral complexes remains, however, an enigma. On one hand, smectite layers composing the clay fraction are known to have a major influence on available surface area. OM maturation occurs, on the other hand, concurrently with the smectite illitization that provokes the closure of the interlayer spaces. The potential of smectite layers in the sequestration and preservation of organic molecules and the fate of these molecules with respect to the smectite illitization were therefore addressed. Here, the mineralogy of three organic-rich source rocks of various maturities was characterized in regards with the geochemistry of their OM. A thorough examination of the clay minerals present in the clay matrices provided evidences of mixed layer minerals containing smectite and illite layers with an increasing illite component with respect to maturity. The comprehensive interpretation of the X-ray diffractograms and analytical electron microscopy results suggested the presence of organic molecules in the inter-particulate and possibly the interlayer spaces of the smectite-rich components in immature source rocks. This eventuality was further supported by the presence of intercalated clay-organic nanocomposites observed by transmitted electron microscopy coupled with energy dispersive spectroscopy. Textural observations also showed that the increased illite content found in the overmature sample led to the reorganization of the OM and the clay particles into nano-scale aggregates. These results clarify the geochemical mechanism beyond the reported relationship between TOC and MSA and allow generalizing it to various organic-rich source rocks. Eventually, the understanding of the close organo-clay association raises prospects on the prediction of the evolution of the mechanical properties of economically valuable source rocks with respect to maturity.