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Molecular complexes of Lewis acid–base pairs can be used to activate molecular hydrogen for applications ranging from hydrogenstorage for fuelcells to catalytichydrogenation reactions. In this paper, we examine the factors that determine the thermodynamics of hydrogenactivation of a Lewis acid–base pair using the pedagogical examples of ammoniaborane (NH3BH3, AB) and ammonium borohydride ([NH4][BH4], ABH2). At ambient temperatures, ABH2 loses hydrogen to form the Lewis acid–base complex AB, suggesting that free energy drives the reaction to release hydrogen. However, direct measurement of the reaction enthalpy is not straightforward given the complex decomposition pathways leading to the formation of the diammoniate of diborane ([NH3BH2NH3][BH4], DADB). In this work, we compare two approaches for deriving the thermodynamic relationships among AB, DADB, and ABH2.
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