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Using the TMG<jats:sub>3<\/jats:sub>tren co\u2010ligand, we have prepared a high\u2010spin ferric NO adduct ({FeNO}<jats:sup>6<\/jats:sup> complex) via electrochemical or chemical oxidation of the corresponding high\u2010spin ferrous NO {FeNO}<jats:sup>7<\/jats:sup> complex. The {FeNO}<jats:sup>6<\/jats:sup> compound is characterized by UV\/Visible and IR spectroelectrochemistry, M\u00f6ssbauer and NMR spectroscopy, X\u2010ray crystallography, and DFT calculations. The data show that its electronic structure is best described as a high\u2010spin iron(IV) center bound to a triplet NO<jats:sup>\u2212<\/jats:sup> ligand with a very covalent iron\u2212NO bond. This finding demonstrates that this high\u2010spin iron nitrosyl compound undergoes iron\u2010centered redox chemistry, leading to fundamentally different properties than corresponding low\u2010spin compounds, which undergo NO\u2010centered redox transformations.<\/jats:p>","DOI":"10.1002\/anie.201601742","type":"journal-article","created":{"date-parts":[[2016,4,22]],"date-time":"2016-04-22T00:55:34Z","timestamp":1461286534000},"page":"6685-6688","source":"Crossref","is-referenced-by-count":47,"title":["Structural and Spectroscopic Characterization of a High\u2010Spin {FeNO}<sup>6<\/sup> Complex with an Iron(IV)\u2212NO<sup>\u2212<\/sup> Electronic Structure"],"prefix":"10.1002","volume":"55","author":[{"given":"Amy L.","family":"Speelman","sequence":"first","affiliation":[{"name":"Department of Chemistry University of Michigan  930 N University Avenue Ann Arbor MI 48109 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Bo","family":"Zhang","sequence":"additional","affiliation":[{"name":"Department of Chemistry, Department of Biochemistry and Molecular Biology The Pennsylvania State University  University Park PA 16802 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Carsten","family":"Krebs","sequence":"additional","affiliation":[{"name":"Department of Chemistry, Department of Biochemistry and Molecular Biology The Pennsylvania State University  University Park PA 16802 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Nicolai","family":"Lehnert","sequence":"additional","affiliation":[{"name":"Department of Chemistry University of Michigan  930 N University Avenue Ann Arbor MI 48109 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2016,4,21]]},"reference":[{"key":"e_1_2_2_1_1","volume-title":"Nitric Oxide: Biology and Pathobiology","year":"2010"},{"key":"e_1_2_2_2_1","unstructured":"\u00a0"},{"key":"e_1_2_2_3_2","doi-asserted-by":"publisher","DOI":"10.1007\/430_2013_92"},{"key":"e_1_2_2_4_2","doi-asserted-by":"publisher","DOI":"10.1016\/j.jinorgbio.2004.10.002"},{"key":"e_1_2_2_5_1","doi-asserted-by":"publisher","DOI":"10.1016\/S0010-8545(00)80259-3"},{"key":"e_1_2_2_6_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja0719982"},{"key":"e_1_2_2_7_1","unstructured":"Two other {FeNO}6complexes have been suggested to be paramagnetic (S=1) but in these cases the proposed spin state was not proven experimentally.[6]"},{"key":"e_1_2_2_8_1","unstructured":"\u00a0"},{"key":"e_1_2_2_9_2","doi-asserted-by":"publisher","DOI":"10.1021\/ic902220a"},{"key":"e_1_2_2_10_2","doi-asserted-by":"publisher","DOI":"10.1039\/c2cc37221e"},{"key":"e_1_2_2_11_1","unstructured":"\u00a0"},{"key":"e_1_2_2_12_2","doi-asserted-by":"publisher","DOI":"10.1002\/anie.200900863"},{"key":"e_1_2_2_12_3","doi-asserted-by":"publisher","DOI":"10.1002\/ange.200900863"},{"key":"e_1_2_2_13_2","doi-asserted-by":"publisher","DOI":"10.1021\/ja100366c"},{"key":"e_1_2_2_14_2","doi-asserted-by":"publisher","DOI":"10.1021\/ic102094d"},{"key":"e_1_2_2_15_2","doi-asserted-by":"publisher","DOI":"10.1073\/pnas.1212693109"},{"key":"e_1_2_2_16_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201305291"},{"key":"e_1_2_2_16_2","doi-asserted-by":"publisher","DOI":"10.1002\/ange.201305291"},{"key":"e_1_2_2_17_1","doi-asserted-by":"publisher","DOI":"10.1021\/ic011243a"},{"key":"e_1_2_2_18_1","unstructured":"Experimental details for the acquisition of crystal data and structure refinement can be found in the Supporting Information. 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