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Oxidation with two equivalents of the ferrocenium salt, [Fe(Cp)<jats:sub>2<\/jats:sub>](BArF<jats:sub>24<\/jats:sub>), affords the dicationic tricarbonyl complex [Fe(CO)<jats:sub>3<\/jats:sub>\u2010\u03b7<jats:sup>4<\/jats:sup>\u2010{(IPr)<jats:sub>2<\/jats:sub>C<jats:sub>2<\/jats:sub>P<jats:sub>2<\/jats:sub>}](BArF<jats:sub>24<\/jats:sub>)<jats:sub>2<\/jats:sub> (<jats:bold>4<\/jats:bold>). The one\u2010electron oxidation proceeds under concomitant loss of one CO ligand to give the paramagnetic dicarbonyl radical cation complex [Fe(CO)<jats:sub>2<\/jats:sub>\u2010\u03b7<jats:sup>4<\/jats:sup>\u2010{(IPr)<jats:sub>2<\/jats:sub>C<jats:sub>2<\/jats:sub>P<jats:sub>2<\/jats:sub>}](BArF<jats:sub>24<\/jats:sub>) (<jats:bold>5<\/jats:bold>). Reduction of <jats:bold>5<\/jats:bold> allows the preparation of the neutral dicarbonyl complex [Fe(CO)<jats:sub>2<\/jats:sub>\u2010\u03b7<jats:sup>4<\/jats:sup>\u2010{(IPr)<jats:sub>2<\/jats:sub>C<jats:sub>2<\/jats:sub>P<jats:sub>2<\/jats:sub>}] (<jats:bold>6<\/jats:bold>). An analysis by various spectroscopic techniques (<jats:sup>57<\/jats:sup>Fe M\u00f6ssbauer, EPR) combined with DFT calculations gives insight into differences of the electronic structure within the members of this unique series of iron carbonyl complexes, which can be either described as electron precise or Wade\u2013Mingos clusters.<\/jats:p>","DOI":"10.1002\/anie.202205371","type":"journal-article","created":{"date-parts":[[2022,6,4]],"date-time":"2022-06-04T14:14:42Z","timestamp":1654352082000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":16,"title":["Bis(imidazolium)\u20101,3\u2010diphosphete\u2010diide: A Building Block for FeC<sub>2<\/sub>P<sub>2<\/sub> Complexes and Clusters"],"prefix":"10.1002","volume":"61","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-4852-065X","authenticated-orcid":false,"given":"Moritz Theodor","family":"Scharnh\u00f6lz","sequence":"first","affiliation":[{"name":"Department of Chemistry and Applied Biosciences ETH Z\u00fcrich  Vladimir-Prelog-Weg 1 8093 Z\u00fcrich Switzerland"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1387-4148","authenticated-orcid":false,"given":"Peter","family":"Coburger","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Applied Biosciences ETH Z\u00fcrich  Vladimir-Prelog-Weg 1 8093 Z\u00fcrich Switzerland"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4241-153X","authenticated-orcid":false,"given":"Lisa","family":"Gravogl","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Pharmacy Inorganic Chemistry Friedrich-Alexander-Universit\u00e4t Erlangen-N\u00fcrnberg (FAU)  Egerlandstr. 1 91058 Erlangen Germany"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3597-0889","authenticated-orcid":false,"given":"Daniel","family":"Klose","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Applied Biosciences ETH Z\u00fcrich  Vladimir-Prelog-Weg 1 8093 Z\u00fcrich Switzerland"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1171-6886","authenticated-orcid":false,"given":"Juan Jos\u00e9","family":"Gamboa\u2010Carballo","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Applied Biosciences ETH Z\u00fcrich  Vladimir-Prelog-Weg 1 8093 Z\u00fcrich Switzerland"},{"name":"Higher Institute of Technologies and Applied Sciences (InSTEC) University of Havana  Ave. S. 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