Synthesis and characterization of a formal 21-electron cobaltocene derivative

Satoshi Takebayashi (), Jama Ariai, Urs Gellrich (), Sergey V. Kartashov, Robert R. Fayzullin (), Hyung-Been Kang, Takeshi Yamane, Kenji Sugisaki and Kazunobu Sato
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Satoshi Takebayashi: Okinawa Institute of Science and Technology Graduate University
Jama Ariai: Justus Liebig University Giessen
Urs Gellrich: Justus Liebig University Giessen
Sergey V. Kartashov: FRC Kazan Scientific Center, Russian Academy of Sciences
Robert R. Fayzullin: FRC Kazan Scientific Center, Russian Academy of Sciences
Hyung-Been Kang: Okinawa Institute of Science and Technology Graduate University
Takeshi Yamane: Osaka Metropolitan University
Kenji Sugisaki: Osaka Metropolitan University
Kazunobu Sato: Osaka Metropolitan University

Nature Communications, 2023, vol. 14, issue 1, 1-10

Abstract: Abstract Metallocenes are highly versatile organometallic compounds. The versatility of the metallocenes stems from their ability to stabilize a wide range of formal electron counts. To date, d-block metallocenes with an electron count of up to 20 have been synthesized and utilized in catalysis, sensing, and other fields. However, d-block metallocenes with more than formal 20-electron counts have remained elusive. The synthesis and isolation of such complexes are challenging because the metal–carbon bonds in d-block metallocenes become weaker with increasing deviation from the stable 18-electron configuration. Here, we report the synthesis, isolation, and characterization of a 21-electron cobaltocene derivative. This discovery is based on the ligand design that allows the coordination of an electron pair donor to a 19-electron cobaltocene derivative while maintaining the cobalt–carbon bonds, a previously unexplored synthetic approach. Furthermore, we elucidate the origin of the stability, redox chemistry, and spin state of the 21-electron complex. This study reveals a synthetic method, structure, chemical bonding, and properties of the 21-electron metallocene derivative that expands our conceptual understanding of d-block metallocene chemistry. We expect that this report will open up previously unexplored synthetic possibilities in d-block transition metal chemistry, including the fields of catalysis and materials chemistry.

Date: 2023
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DOI: 10.1038/s41467-023-40557-7

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