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Using sterically demanding pentafulvenes gives a clean exchange reaction, yielding vanadium pentafulvene (<jats:bold>2<\/jats:bold>\u2009<jats:bold>a<\/jats:bold> and <jats:bold>2<\/jats:bold>\u2009<jats:bold>b<\/jats:bold>) and benzofulvene complexes (<jats:bold>3<\/jats:bold>\u2009<jats:bold>a<\/jats:bold> and <jats:bold>3<\/jats:bold>\u2009<jats:bold>b<\/jats:bold>). The molecular structures of the target compounds suggest a \u03c0\u2010\u03b7<jats:sup>5<\/jats:sup>:\u03c3\u2010\u03b7<jats:sup>1<\/jats:sup> coordination mode with a vanadium<jats:sup>III<\/jats:sup> center. With the sterically low demanding 6,6\u2010dimethylpentafulvene, a C\u2212H activation at the leaving ligand is observed, yielding the ring\u2010substituted vanadocene<jats:sup>II<\/jats:sup> <jats:bold>4<\/jats:bold>. The reactivity of the pentafulvene complexes was investigated. A series of unprecedented vanadocene<jats:sup>III<\/jats:sup> compounds were synthesized: Under mild conditions, E\u2212H splitting of 4\u2010<jats:italic>tert\u2010<\/jats:italic>butylphenol, diphenylamine, and 2,6\u2010diisopropylaniline yield well characterized examples of rare vanadocene<jats:sup>III<\/jats:sup> phenolate and amide complexes. Insertion reactions into the V\u2212C<jats:sub>exo<\/jats:sub> bond of the pentafulvene complexes by multiple bond containing substrates were found for acetone, 4\u2010chlorobenzonitril and <jats:italic>N<\/jats:italic>,<jats:italic>N\u2019<\/jats:italic>\u2010dicyclohexylcarbodiimide.<\/jats:p>","DOI":"10.1002\/chem.202203846","type":"journal-article","created":{"date-parts":[[2023,3,9]],"date-time":"2023-03-09T10:48:40Z","timestamp":1678358920000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":4,"title":["Vanadium Pentafulvene Complexes: Synthon for Unprecedented Vanadocene<sup>III<\/sup> Derivatives"],"prefix":"10.1002","volume":"29","author":[{"given":"Simon","family":"de Graaff","sequence":"first","affiliation":[{"name":"Institut f\u00fcr Chemie Carl von Ossietzky Universit\u00e4t Oldenburg  26111 Oldenburg Germany"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Kevin","family":"Schwitalla","sequence":"additional","affiliation":[{"name":"Institut f\u00fcr Chemie Carl von Ossietzky Universit\u00e4t Oldenburg  26111 Oldenburg Germany"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Hermann","family":"Thye","sequence":"additional","affiliation":[{"name":"Institut f\u00fcr Chemie Carl von Ossietzky Universit\u00e4t Oldenburg  26111 Oldenburg Germany"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Zainab","family":"Yusufzadeh","sequence":"additional","affiliation":[{"name":"Institut f\u00fcr Chemie Carl von Ossietzky Universit\u00e4t Oldenburg  26111 Oldenburg Germany"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Michael","family":"Willms","sequence":"additional","affiliation":[{"name":"Institut f\u00fcr Chemie Carl von Ossietzky Universit\u00e4t Oldenburg  26111 Oldenburg Germany"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8026-7271","authenticated-orcid":false,"given":"Marc","family":"Schmidtmann","sequence":"additional","affiliation":[{"name":"Institut f\u00fcr Chemie Carl von Ossietzky Universit\u00e4t Oldenburg  26111 Oldenburg Germany"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3697-0378","authenticated-orcid":false,"given":"R\u00fcdiger","family":"Beckhaus","sequence":"additional","affiliation":[{"name":"Institut f\u00fcr Chemie Carl von Ossietzky Universit\u00e4t Oldenburg  26111 Oldenburg Germany"}],"role":[{"role":"author","vocabulary":"crossref"}]}],"member":"311","published-online":{"date-parts":[[2023,4,12]]},"reference":[{"key":"e_1_2_8_1_1","unstructured":"\u00a0"},{"key":"e_1_2_8_2_2","doi-asserted-by":"publisher","DOI":"10.1007\/BF00617242"},{"key":"e_1_2_8_3_2","doi-asserted-by":"publisher","DOI":"10.1021\/ja01646a008"},{"key":"e_1_2_8_4_2","doi-asserted-by":"publisher","DOI":"10.1515\/znb-1954-0722"},{"key":"e_1_2_8_5_1","unstructured":"\u00a0"},{"key":"e_1_2_8_6_2","doi-asserted-by":"crossref","unstructured":"T.\u2005S. 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