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Plasma Treated-Ultrathin Ternary FePSe3 Nanosheets as a Bifunctional Electrocatalyst for Efficient Zinc-Air Batteries.

Developing novel bifunctional electrocatalysts with advanced oxygen electrocatalytic activity is pivotal for next-generation energy-storage devices. Herein, we present an ultrathin oxygen doped FePSe3 (FePSe3-O) nanosheets by the Ar/O2 plasma treatment with remarkable surface atom reorganization. Such surface atom reorganization generates multiple crystalline-amorphous interfaces that benefit the kinetics of oxygen evolution reaction, achieving a low overpotential of only 261 mV at 10 mA cm2 with a small Tafel slope of 41.13 mV dec1. Density functional theory calculation indicates that the oxygen doping can also modulate the electrical states at the Fermi level with a decreased band gap responsible for the enhanced electrocatalytic performance. Such unique FePSe3-O nanosheets can be further fabricated as the air cathode in rechargeable liquid zinc-air batteries (ZABs), which deliver a high open circuit potential of 1.47 V, a small charge-discharge voltage gap of 0.80 V, and good cycling stability for more than 800 circles. As a proof of concept, the flexible solid-state ZABs assembled with FePSe3-O nanosheets cathode also display a favorable charge-discharge performance, durable stability, and good bendability. This work sheds new insight into the rational design of defect-rich ternary thiophosphate nanosheets by plasma treatment towards enhanced oxygen electrocatalysts in metal-air batteries.