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Finding proper electrocatalysts capable of efficient catalyzing both ORR andOER is of great importance for metal-air batteries. With increasing inclinationtowards structural and flexible devices, developing a high-performanceself-standing air-cathode is highly demanded and challenging, as most of oxygencatalysts are powder and need to be further processed. Here, we constructhighly bifunctional air catalyst from macroscopic CNT fibers (CNTf) throughdirect CVD spinning followed by hydrothermal method. The electrocatalyticproperties of the samples were tuned by altering nitrogen-doping and defectdensities readily adjusted at different hydrothermal reaction temperatures. Thetreated CNTfs showed excellent bifunctional activity ({\Delta}E=Ej=10-E1/2=0.81V) and demonstrated exceptional performance as carbon-based self-standingair-cathodes in liquid and solid-state rechargeable Zn-air batteries, with highcapacity of 698 mAh g-1 and ultrahigh energy density of 838 Wh kg-1. Therechargeable Zn-air batteries exhibit a low discharge-charge overpotential andexcellent stability. This work provides novel simply achieved self-standing airelectrodes with exceptional performance for structural Zn-air batteries.

Doping of Self-Standing CNT Fibers: Promising Flexible Air-Cathodes for High Energy Density Structural Zn-air batteries