"Ship in a Bottle" Design of Highly Efficient Bifunctional Electrocatalysts for Long-Lasting Rechargeable Zn-Air Batteries.

Abstract

The poor durability of bifunctional oxygen electrocatalysts is one main bottleneck that suppresses the widespread application of rechargeable metal-air batteries. Herein, a "ship in a bottle" design is achieved by impregnating fine transition metal dichalcogenide nanoparticles into defective carbon pores that act as interconnected nanoreactors. The erected 3D porous conductive architecture provides a "highway" for expediting charge and mass transfer. This design not only delivers a high surface-to-volume ratio to increase numbers of exposed catalytic sites but also precludes nanoparticles from aggregation during cycling owing to the pore spatial confinement effect. Therefore, the long-term plague inherent to nanocatalyst stability can be solved. Moreover, the synergistic coupling effects between defect-rich interfaces and chemical bonding derived from heteroatom-doping boost the catalytic activity and prohibit the detachment of nanoparticles for better stability. Consequently, the developed catalyst presents superior bifunctional oxygen electrocatalytic activities and durability, out-performing the best-known noble-metal benchmarks. In a practical application to rechargeable Zn-air batteries, long-term cyclability for over 340 h is realized at a high current density of 25 mA cm^-2 in ambient air while retaining an intact structure. Such a universal "ship in a bottle" design offers an appealing and instructive model of nanomaterial engineering for implementation in various fields.