Redox-Based Spin Diversity in a 6-Oxophenalenoxyl System: Generation, ESR/ENDOR/TRIPLE, and Theoretical Studies of 2,5,8-Tri-<i>tert</i>-butylphenalenyl- 1,6-bis(olate) Salts

Abstract

[reaction: see text] Novel open-shell molecular salts, 2,5,8-tri-tert-butylphenalenyl-1,6-bis(olate) salts, were designed on the basis of the 6-oxophenalenoxyl system and generated by the chemical reduction of 6-hydroxyphenalenone derivatives. ESR/ENDOR/TRIPLE measurements and DFT calculations provide unequivocal determination of the structure and spin density distribution, which demonstrate redox-based spin diversity of the 6-oxophenalenoxyl system.