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Experimental study demonstrates efficient aqueous nitrile hydrolysis using a graphene oxide-supported ruthenium catalyst, indicating high reusability and selectivity for green chemical synthesis.
A ruthenium-dmso catalyst was heterogenized on graphene oxide (GO) for the first time, providing a sustainable system for nitrile hydrolysis in water. Three isomers of the [RuCl2(bpea-pyrene)(dmso)] complex, trans,mer-2a (2a), trans,fac-2b (2b), and cis,fac- 2c (2c) (bpea-pyrene = 1-[bis(pyridine-2-ylmethyl)amino]methylpyrene; dmso = dimethyl sulfoxide), were synthesized and characterized. Isomerization studies supported by DFT calculations confirmed that 2c is the thermodynamically most stable isomer and elucidated the pathways connecting 2a, 2b, and 2c. Photo- and thermochemically induced processes were investigated in various solvents, revealing distinct ligand substitution and oxidation pathways. Isomer 2c was heterogenized on GO via π–π interactions between the pyrene unit and the support, representing the first example of a molecular Ru-dmso complex noncovalently anchored on GO. Both homogeneous 2c and heterogeneous GO@2c efficiently catalyzed the transformation of nitriles to amides with high selectivity under aqueous conditions. The supported catalyst showed enhanced activity toward acrylonitrile, excellent reusability over five consecutive runs, negligible Ru leaching, and high structural stability. These findings establish GO@2c as an efficient, reusable, and sustainable catalyst for aqueous nitrile hydrolysis, and a plausible catalytic mechanism is proposed.
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Roca et al. (2026) studied this question.
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