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Aerobic iron-catalyzed site-selective C(sp3)–C(sp3) bond cleavage in N-heterocycles
2021, Leonard, David K., Li, Wu, Rockstroh, Nils, Junge, Kathrin, Beller, Matthias
The kinetic and thermodynamic stability of C(sp3)–C(sp3) bonds makes the site-selective activation of these motifs a real synthetic challenge. In view of this, herein a site-selective method of C(sp3)–C(sp3) bond scission of amines, specifically morpholine and piperazine derivatives, using a cheap iron catalyst and air as a sustainable oxidant is reported. Furthermore, a statistical design of experiments (DoE) is used to evaluate multiple reaction parameters thereby allowing for the rapid development of a catalytic process. © 2021
Cobalt-Catalyzed Aqueous Dehydrogenation of Formic Acid
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.