Metal–organic framework (MOF)‐derived Co‐N‐C catalysts with isolated single cobalt atoms have been synthesized and compared with cobalt nanoparticles for formic acid dehydrogenation. The atomically dispersed Co‐N‐C catalyst achieves superior activity, better acid resistance, and improved long‐term stability compared with nanoparticles synthesized by a similar route. High‐angle annular dark‐field–scanning transmission electron microscopy, X‐ray photoelectron spectroscopy, electron paramagnetic resonance, and X‐ray absorption fine structure characterizations reveal the formation of CoIINx centers as active sites. The optimal low‐cost catalyst is a promising candidate for liquid H2 generation.

Hydrodehalogenation is an effective strategy for transforming persistent and potentially toxic organohalides into their more benign congeners. Common methods utilize Pd/C or Raney‐nickel as catalysts, which are either expensive or have safety concerns. In this study, a nickel‐based catalyst supported on titania (Ni‐phen@TiO2‐800) is used as a safe alternative to pyrophoric Raney‐nickel. The catalyst is prepared in a straightforward fashion by deposition of nickel(II)/1,10‐phenanthroline on titania, followed by pyrolysis. The catalytic material, which was characterized by SEM, TEM, XRD, and XPS, consists of nickel nanoparticles covered with N‐doped carbon layers. By using design of experiments (DoE), this nanostructured catalyst is found to be proficient for the facile and selective hydrodehalogenation of a diverse range of substrates bearing C−I, C−Br, or C−Cl bonds (>30 examples). The practicality of this catalyst system is demonstrated by the dehalogenation of environmentally hazardous and polyhalogenated substrates atrazine, tetrabromobisphenol A, tetrachlorobenzene, and a polybrominated diphenyl ether (PBDE).

Cobalt‐doped hybrid materials consisting of metal oxides and carbon derived from chitin were prepared, characterized and tested for industrially relevant nitrile hydrogenations. The optimal catalyst supported onto MgO showed, after pyrolysis at 700 °C, magnesium oxide nanocubes decorated with carbon‐enveloped Co nanoparticles. This special structure allows for the selective hydrogenation of diverse and demanding nitriles to the corresponding primary amines under mild conditions (e.g. 70 °C, 20 bar H2). The advantage of this novel catalytic material is showcased for industrially important substrates, including adipodinitrile, picolinonitrile, and fatty acid nitriles. Notably, the developed system outperformed all other tested commercial catalysts, for example, Raney Nickel and even noble‐metal‐based systems in these transformations.