0000000001308100
AUTHOR
Vega Lloveras
Organic Polyradicals as Redox Mediators: Effect of Intramolecular Radical Interactions on Their Efficiency
The spin–spin interactions between unpaired electrons in organic (poly)radicals, especially nitroxides, are largely investigated and are of crucial importance for their applications in areas such as organic magnetism, molecular charge transfer, or multiple spin labeling in structural biology. Recently, 2,2,6,6-tetramethylpiperidinyloxyl and polymers functionalized with nitroxides have been described as successful redox mediators in several electrochemical applications; however, the study of spin–spin interaction effect in such an area is absent. This communication reports the preparation of a novel family of discrete polynitroxide molecules, with the same number of radical units but differe…
Allocation of Ambipolar Charges on an Organic Diradical with a Vinylene-Phenylenediyne Bridge.
Two redox and magnetically active perchlorotriphenylmethyl (• PTM) radical units have been connected as end-capping groups to a bis(phenylene)diyne chain through vinylene linkers. Negative and positive charged species have been generated, and the influence of the bridge on their stabilization is discussed. Partial reduction of the electron-withdrawing • PTM radicals results in a class-II mixed-valence system with the negative charge located on the terminal PTM units, proving the efficiency of the conjugated chain for the electron transport between the two terminal sites. Counterintuitively, the oxidation process does not occur along the electron-rich bridge but on the vinylene units. The • …
Tetrathiafulvalene-Based Mixed-Valence Acceptor-Donor-Acceptor Triads: A Joint Theoretical and Experimental Approach
This work presents a joint theoretical and experimental characterisation of the structural and electronic properties of two tetrathiafulvalene (TTF)-based acceptor-donor-acceptor triads (BQ-TTF-BQ and BTCNQ-TTF - BTCNQ; BQ is naphthoquinone and BTCNQ is benzotetracyano-p-quinodimethane) in their neutral and reduced states. The study is performed with the use of electrochemical, electron paramagnetic resonance (EPR), and UV/Vis/NIR spectroelectrochemical techniques guided by quantum-chemical calculations. Emphasis is placed on the mixed-valence properties of both triads in their radical anion states. The electrochemical and EPR results reveal that both BQ-TTF-BQ and BTCNQ-TTF-BTCNQ triads in…
Dibenzocycloheptatriene as end-group of Thiele and tetrabenzo-Chichibabin hydrocarbons
The authors are grateful for the financial support from: MICIU/FEDER/AEI, Spain (PG2018-101181-B-I00, PGC2018-095808B-I00, MAT2016-80826-R, FIP-2018-HECTIC-PTM, Prometeo2019/076 and the "Severo Ochoa" Programme for Centres of Excellence in R & D; SEV-2015-0496), the European Research Council (ERC) (677023), DGR (Catalunya) (2017-SGR-918), and SNSF (Switzerland, TS., PZ00P2_174175). We thank the CSIRC-Alhambra and SciCore (Basel, Switzerland) for supercomputing facilities and the Servei de RMN, UAB, for instrument time.
CCDC 1986124: Experimental Crystal Structure Determination
Related Article: Elena Badetti, Vega Lloveras, Emanuele Amadio, Rosalia Di Lorenzo, Mara Olivares-Marín, Alvaro Y. Tesio, Songbai Zhang, Fangfang Pan, Kari Rissanen, Jaume Veciana, Dino Tonti, Jose Vidal-Gancedo, Cristiano Zonta, Giulia Licini|2020|ACS Applied Materials and Interfaces|12|45968|doi:10.1021/acsami.0c09386
CCDC 2012097: Experimental Crystal Structure Determination
Related Article: Vicente G. Jiménez, Paula Mayorga-Burrezo, Victor Blanco, Vega Lloveras, Carlos J. Gómez-García, Tomáš Šolomek, Juan M. Cuerva, Jaume Veciana, Araceli G. Campaña|2020|Chem.Commun.|56|12813|doi:10.1039/D0CC04489J
CCDC 2012098: Experimental Crystal Structure Determination
Related Article: Vicente G. Jiménez, Paula Mayorga-Burrezo, Victor Blanco, Vega Lloveras, Carlos J. Gómez-García, Tomáš Šolomek, Juan M. Cuerva, Jaume Veciana, Araceli G. Campaña|2020|Chem.Commun.|56|12813|doi:10.1039/D0CC04489J