Octahedral Cobalt(III) Complex Based on Cheap 1,2-Phenylenediamine as a Bifunctional Metal-Templated Hydrogen Bond Donor Catalyst for Fixation of CO2 with Epoxides at Ambient Conditions

Емельянов, М.А.; Stoletova, N.V.; Lisov, A.A.; Medvedev, M.G.; Smolyakov, A.F.; Maleev, V.I.; Larionov, V.A.

Статья опубликована в высокорейтинговом журнале

Информация о цитировании статьи получена из Web of Science
Статья опубликована в журнале из списка Web of Science и/или Scopus
Дата последнего поиска статьи во внешних источниках: 8 сентября 2021 г.

Авторы: Емельянов Михаил А., Stoletova Nadezhda V., Lisov Alexey A., Medvedev M.G., Smolyakov A.F., Maleev Victor I., Larionov Vladimir A.
Журнал: INORGANIC CHEMISTRY FRONTIERS
Том: 8
Номер: 16
Год издания: 2021
Первая страница: 3871
Последняя страница: 3884
DOI: 10.1039/d1qi00464f
Аннотация: Hydrogen bond donors (HBD) are a sustainable privileged class of catalysts which are broadly used for the activation of compounds in synthetic chemistry. Among them, the metal-templated HBD complexes present perspective systems with high catalytic potential. In this respect, here we report the design of the next-generation octahedral Co(III) complexes based on cheap commercially available 1,2-phenylenediamine and 3,5-di-tert-butyl-salicylaldehyde. It was shown that the obtained Co(III) complex with an iodide counter-anion operates as a bifunctional one-component hydrogen bond donor/nucleophilic catalyst for the fixation of carbon dioxide with epoxides into valuable cyclic carbonates at ambient conditions (RT and 1 bar CO2) under solvent and co-catalyst free conditions. The TON and TOF values of 38 and 1.6, respectively, were achieved at low catalyst loading (2 mol%) under ambient conditions. Furthermore, the obtained Co(III) complex catalyzed the reaction with diluted air/CO2 mixture (15 vol% of CO2) producing the desired cyclic carbonate in a 92% yield. A plausible catalytic cycle consistent with all experimental observations was proposed based on DFT calculations. The epoxide-opening step was found to be the rate-determining. Besides, the influence of different additives on the catalysis was investigated and explained computationally.
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