An n-Type Open-Shell Conjugated Polymer with High-Spin Ground-State and High Intrinsic Electrical Conductivity.
Angew Chem Int Ed Engl
; 63(25): e202402375, 2024 Jun 17.
Article
em En
| MEDLINE
| ID: mdl-38619528
ABSTRACT
Open-shell conjugated polymers with a high intrinsic conductivity and high-spin ground state hold considerable promise for applications in organic electronics and spintronics. Herein, two novel acceptor-acceptor (A-A) conjugated polymers based on a highly electron-deficient quinoidal benzodifurandione unit have been developed, namely DPP-BFDO-Th and DPP-BFDO. The incorporation of the quinoidal moiety into the polymers backbones enables deeply aligned lower-lying lowest unoccupied molecular orbital (LUMO) levels of below -4.0â
eV. Notably, DPP-BFDO exhibits an exceptionally low LUMO (-4.63â
eV) and a high-spin ground state characterized by strong diradical characters. Moreover, a self-doping through intermolecular charge-transfer is observed for DPP-BFDO, as evidenced by X-ray photoelectron spectroscopy (XPS) studies. The high carrier concentration in combination with a planar and linear conjugated backbone yields a remarkable electrical conductivity (σ) of 1.04â
S cm-1 in the "undoped" native form, ranking among the highest values reported for n-type radical-based conjugated polymers. When employed as an n-type thermoelectric material, DPP-BFDO achieves a power factor of 12.59â
µW m-1 K-2. Furthermore, upon n-doping, the σ could be improved to 65.68â
S cm-1. This study underscores the great potential of electron-deficient quinoidal units in constructing dopant-free n-type conductive polymers with a high-spin ground state and exceptional intrinsic conductivity.
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MEDLINE
Idioma:
En
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Angew Chem Int Ed Engl
Ano de publicação:
2024
Tipo de documento:
Article