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    Cobalt Single-Atom Catalysts with High Stability for Selective Dehydrogenation of Formic Acid
    (Weinheim : Wiley-VCH, 2020) Li, Xiang; Surkus, Annette-Enrica; Rabeah, Jabor; Anwar, Muhammad; Dastigir, Sarim; Junge, Henrik; Brückner, Angelika; Beller, Matthias
    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. © 2020 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.
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    Cobalt-Catalyzed Aqueous Dehydrogenation of Formic Acid
    (Weinheim : Wiley-VCH, 2019) Zhou, Wei; Wei, Zhihong; Spannenberg, Anke; Jiao, Haijun; Junge, Kathrin; Junge, Henrik; Beller, Matthias
    Among the known liquid organic hydrogen carriers, formic acid attracts increasing interest in the context of safe and reversible storage of hydrogen. Here, the first molecularly defined cobalt pincer complex is disclosed for the dehydrogenation of formic acid in aqueous medium under mild conditions. Crucial for catalytic activity is the use of the specific complex 3. Compared to related ruthenium and manganese complexes 7 and 8, this optimal cobalt complex showed improved performance. DFT computations support an innocent non-classical bifunctional outer-sphere mechanism on the triplet state potential energy surface. © 2019 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.