Therefore, according to the available literature data, the formal electron count of MnCp 2(dmpe) cannot be conclusively described. ![]() The solid-state zigzag chain structure of MnCp 2 is a vivid example of the anomalous coordination chemistry of manganocene complexes 23. This anomalous behavior of manganocene complexes is attributed to the primarily electrostatic character of the Mn–C(Cp) interactions, and the observed coordination modes are mainly controlled by the steric factor of the ligands 22, 23, 24. Furthermore, as with other manganocene complexes, the coordination mode of the Cp ligands in this complex deviates from the ideal η 5-coordination because of ring slippage 15, 17, 18, 19, 20, 21, 22. However, as noted by the authors, the formation of this complex does not follow the expected trend of other metallocenes 16. reported a possible formal 21-electron manganocene derivative, MnCp 2(dmpe) (Fig. To date, d-block metallocenes and their derivatives with a formal electron count in the range from 14 to 20, including recently synthesized 16-electron ferrocene dication 13 and 20-electron cobaltocene anion 14, have been isolated. The versatility of metallocenes stems from the ability of the cyclopentadienyl ligand (Cp) and its derivatives to stabilize metals with a wide range of valence electron counts. 1, and the Nobel Prize-winning work of Fischer and Wilkinson 2, 3, various derivatives of metallocenes have been synthesized and have played pivotal roles in important discoveries in a variety of fields, including catalysis 4, 5, materials 6, 7, 8, 9, energy 10, and medical 11, 12 sciences (Fig. Since the discovery of ferrocene in the 1950s by Kealy and Pauson, as well as Miller et al. 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. 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. Furthermore, we elucidate the origin of the stability, redox chemistry, and spin state of the 21-electron complex. ![]() 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. Here, we report the synthesis, isolation, and characterization of a 21-electron cobaltocene derivative. 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. However, d-block metallocenes with more than formal 20-electron counts have remained elusive. To date, d-block metallocenes with an electron count of up to 20 have been synthesized and utilized in catalysis, sensing, and other fields. The versatility of the metallocenes stems from their ability to stabilize a wide range of formal electron counts. Metallocenes are highly versatile organometallic compounds.
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