Hidden Noninnocence: Theoretical and Experimental Evidence for Redox Activity of a β‐Diketiminate(1−) Ligand

End of innocence: A β-diketiminate(1−) ligand, formerly thought to be innocent, is shown to be redox-active: It can undergo one-electron oxidation to form a neutral π radical stabilized by coordination to a high-spin NiII ion (see scheme). However, since the change in oxidation state of the ligand does not significantly change intraligand bond lengths, its noninnocence is hidden from X-ray crystallography. Detailed facts of importance to specialist readers are published as ”Supporting Information”. Such documents are peer-reviewed, but not copy-edited or typeset. They are made available as submitted by the authors. Please note: The publisher is not responsible for the content or functionality of any supporting information supplied by the authors. Any queries (other than missing content) should be directed to the corresponding author for the article.