Silica nanoparticles (NPs) with fibrous morphology (KCC-1) coated with TiO2 and functionalized with amine chains (KCC-1-TiO2-NH2) are promising materials for the integrated capture of CO2 and its photoconversion into fuels or chemicals. Such nanocatalysts should combine high surface area, high accessibility, efficient CO2 capture and good water stability. However, there are still unsettled questions about the structure and the activity of this type of nanophotocatalysts, including (i) the structure of the TiO2 surface and its interaction with reactants (CO2 and H2O); (ii) the structure of TiO2 phases supported on silica and the SiO2-TiO2 interactions; and (iii) the orientation and the mobility of the grafted amine chains. The EOS project aims at obtaining such information by developing innovative high-field solid-state (DNP)-NMR instruments and methods since this spectroscopy is suited to the characterization of heterogeneous and/or disordered materials. The techniques developed in the project will open new avenues for the detection of insensitive quadrupolar nuclei (47/49Ti, 14N, 17O) near surface. We will notably design innovative instrumentation for the observation of these isotopes using 1.2 GHz NMR spectrometers. We will also explore novel approaches to improve the sensitivity of 800 MHz DNP-NMR. NMR methods will also be introduced to selectively observe the insensitive quadrupolar nuclei near surfaces and to probe their interactions with the reactants (H2O, CO2). These novel (DNP)-NMR techniques will lead to a better understanding of the structure and the dynamcis of KCC-1-TiO2-NH2 surface and its interactions with reactants. This new knowledge will be used to rationally improve the conception of the nanocatalysts and their performances. This project addresses important questions in NMR, heterogeneous catalysis and material sciences. It will open new horizons for the conception of photocatalysts, which is a crucial technology for the clean energy challenge.