Innovative solutions have been designed to meet the global demand for energy and environmental sustainability, such as enhanced hydrocarbon recovery and geo-sequestration of CO 2 . These processes involve the movement of immiscible fluids through permeable rocks, which is affected by the interfacial properties of rocks at the pore scale. Overcoming major challenges in these processes relies on a deeper understanding about the fundamental factors that control the rock wettability. In particular, the efficiency of oil recovery strategies depends largely on the 3D wetting pattern of reservoir rocks, which is in turn affected by the adsorption and deposition of ‘contaminant’ molecules on the pores’ surface. Here, we combined high-resolution neutron tomography (NT) and synchrotron X-ray tomography (XRT) to probe the previously unobserved 3D distribution of molecular and mineralogical heterogeneity of oil reservoir rocks at the pore scale. Retrieving the distribution of neutron attenuation coefficients by Monte Carlo simulations, 3D molecular chemical mappings with micrometer dimensions could be provided. This approach allows us to identify co-localization of mineral phases with chemically distinct hydrogen-containing molecules, providing a solid foundation for the understanding of the interfacial phenomena involved in multiphase fluid flow in permeable media.

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Carbonate and sandstone reservoirs play an important role in oil industry as they host over 50% of the world’s hydrocarbon reserves. For an accurately assessment of porosity and pore size distribution of such complex pore-network, which affect directly the macroscopic characteristics of multiphase fluid flow, X-ray computed microtomography (micro-CT) emerges as a powerful tool. In contrast to lab-based X-ray micro-CT (XCT), synchrotron X-ray micro-CT (SXCT) images are commonly free of artefacts (i.e. beam hardening) and the unique properties of synchrotron sources enable the X-ray imaging of complex and heterogeneous materials in greater detail, with higher quality, and short acquisition time. This work reports results of cone beam computed microtomography (XCT) in comparison with synchrotron computed microtomography (SXCT) applied to very heterogeneous carbonate and sandstone reservoir rocks. We analyze the quality of the image generated in terms of detection of details and artefacts, the advantages and limitation of each technique, as well as features like contrast, sharpness, and signal-to-noise ratio (SNR). Although SXCT offers significant advantages over XCT, the latter gains in cost of operation, accessibility and user-friendliness.