Tandem Dehydrogenation of Ammonia Borane and Hydrogenation of Nitro/Nitrile Compounds Catalyzed by Graphene-Supported NiPd Alloy Nanoparticles

Metin, Onder/0000-0003-1622-4992; Mendoza-Garcia, Adriana/0000-0002-2892-4470WOS: 000337074700016We report a facile synthesis of monodisperse NiPd alloy nanoparticles (NPs) and their assembly on graphene (G) to catalyze the tandem dehydrogenation of ammonia borane (AB) and hydrogenation of R-NO2 and/or R-CN to R-NH2 in aqueous methanol solutions at room temperature. The 3.4 nm NiPd alloy NPs were prepared by coreduction of nickel(II) acetate and palladium(H) acetlyacetonate by borane-tert-butylamine in oleylamine and deposition on G via a solution phase self-assembly process. G-NiPd showed composition-dependent catalysis on the tandem reaction with G-Ni30Pd70 being the most active. A variety of R-NO2 and/or R-CN derivatives were reduced selectively into R-NH2 via G-Ni30Pd70 catalyzed tandem reaction in 5-30 mm reaction time with the conversion yields reaching up to 100%. Our study demonstrates a new approach to G-NiPd-catalyzed dehydrogenation of AB and hydrogenation of R-NO2 and R-CN. The G-NiPd NP catalyst is efficient and reusable, and the reaction can be performed in an environment-friendly process with short reaction times and high yields.Scientific and Technological Research Council of Turkey (TUBITAK)Turkiye Bilimsel ve Teknolojik Arastirma Kurumu (TUBITAK) [113Z276]; U.S. Army Research LaboratoryUnited States Department of DefenseUS Army Research Laboratory (ARL); U.S. Army Research Office under the Multi University Research Initiative (MURI)MURI [W911NF-11-1-0353]This work was supported by the Scientific and Technological Research Council of Turkey (TUBITAK, Project No: 113Z276), the U.S. Army Research Laboratory, and the U.S. Army Research Office under the Multi University Research Initiative (MURI, grant number W911NF-11-1-0353) on "Stress-Controlled Catalysis via Engineered Nanostructures.

Tandem Dehydrogenation of Ammonia Borane and Hydrogenation of Nitro/Nitrile Compounds Catalyzed by Graphene-Supported NiPd Alloy Nanoparticles

We report a facile synthesis of monodisperse NiPd alloy nanoparticles (NPs) and their assembly on graphene (G) to catalyze the tandem dehydrogenation of ammonia borane (AB) and hydrogenation of R-NO₂ and/or R-CN to R-NH₂ in aqueous methanol solutions at room temperature. The 3.4 nm NiPd alloy NPs were prepared by coreduction of nickel­(II) acetate and palladium­(II) acetlyacetonate by borane-<i>tert</i>-butylamine in oleylamine and deposition on G via a solution phase self-assembly process. G-NiPd showed composition-dependent catalysis on the tandem reaction with G-Ni₃₀Pd₇₀ being the most active. A variety of R-NO₂ and/or R-CN derivatives were reduced selectively into R-NH₂ via G-Ni₃₀Pd₇₀ catalyzed tandem reaction in 5–30 min reaction time with the conversion yields reaching up to 100%. Our study demonstrates a new approach to G-NiPd-catalyzed dehydrogenation of AB and hydrogenation of R-NO₂ and R-CN. The G-NiPd NP catalyst is efficient and reusable, and the reaction can be performed in an environment-friendly process with short reaction times and high yields