Fernández Bartolomé, EstefaníaGamonal, ArturoSantos Barahona, José ManuelKhodabakhshi, SaeedRodríguez Sánchez, EiderSañudo, CarolinaMartín León, NazarioSánchez Costa, José2024-01-162024-01-162021Fernandez-Bartolome, E.; Gamonal, A.; Santos, J.; Khodabakhshi, S.; Rodríguez-Sánchez, E.; Sañudo, E. C.; Martín, N.; Sánchez Costa, J. Playing with the weakest supramolecular interactions in a 3D crystalline hexakis[60]fullerene induces control over hydrogenation selectivity. Chem. Sci. 2021, 12, 8682-8688 DOI:10.1039/D1SC00981H.2041-652010.1039/d1sc00981hhttps://hdl.handle.net/20.500.14352/93427Weak forces can play an essential role in chemical reactions. Controlling such subtle forces in reorganization processes by applying thermal or chemical stimuli represents a novel synthetic strategy and one of the main targets in supramolecular chemistry. Actually, to separate the different supramolecular contributions to the stability of the 3D assemblies is still a major challenge. Therefore, a clear differentiation of these contributions would help in understanding the intrinsic nature as well as the chemical reactivity of supramolecular ensembles. In the present work, a controlled reorganization of an hexakis[60]fullerene-based molecular compound purely governed by the weakest van der Waals interactions known, i.e. the dihydrogen interaction – usually called sticky fingers – is illustrated. This pre-reorganization of the hexakis[60]fullerene under mild conditions allows a further selective hydrogenation of the crystalline material via hydrazine vapors exposure. This unique two-step transformation process is monitored by single-crystal to single-crystal diffraction (SCSC) which allows the direct observation of the molecular movements in the lattice and the subsequent solid–gas hydrogenation reaction.engAttribution-NonCommercial-NoDerivatives 4.0 Internationalhttp://creativecommons.org/licenses/by-nc-nd/4.0/journal article2041-6539https://doi.org/10.1039/d1sc00981hopen access547Química orgánica (Química)2306 Química Orgánica