4.8 Article

Molecular Tailoring of p-type Organics for Zinc Batteries with High Energy Density

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Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202304036

Keywords

Molecular Tailoring; P-Type Organic Cathode; Phenothiazine; Zn-Anode; Zn-Organic Battery

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By combining single-electron and multi-electron units, a new molecule named PTZAN was designed as a high-capacity and stable p-type organic electrode material. The PTZAN-Zn battery exhibited excellent performance with high stability, voltage, capacity, and energy density.
P-type organic electrode materials are known for their high redox voltages and fast kinetics. However, single-electron p-type organic materials generally exhibit low capacity despite high operating voltage and stability, while some multi-electron p-type organic materials have high theoretical capacity but low stability. To address this challenge, we explore the possibility of combining single-electron and multi-electron units to create high-capacity and stable p-type organic electrodes. We demonstrate the design of a new molecule, 4,4 '-(10H-phenothiazine-3,7-diyl) bis (N,N-diphenylaniline) (PTZAN), which is created by coupling the triphenylamine molecule and the phenothiazine molecule. The resulting PTZAN||Zn battery shows excellent stability (2000 cycles), high voltage (1.3 V), high capacity (145 mAh g(-1)), and energy density of 187.2 Wh kg(-1). Theoretical calculations and in/ex situ analysis reveal that the charge storage of the PTZAN electrode is mainly driven by the redox of phenothiazine heterocycles and triphenylamine unit, accompanied by the combination/release of anions and Zn2+.

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