Abstract

Metal-free catalysts are made by the elements with infinite reserve in nature and, therefore, show the potential for large-scale applications in energy devices including metal-air batteries. The construction of metal-air batteries prefers using self-supporting catalysts with favorable activity as well as fast kinetics. However, it is challenging due to the limited electropositivity of metal-free catalysts for O-O bond formation in oxygen evolution reaction (OER), scaling relationship restrictions between OER and oxygen reduction reaction, and difficulty in porosity construction on the monolith electrode surface. In this contribution, through developing a facile methodology of quenching high-temperature carbon clothes in liquid nitrogen, a self-supported carbon cloth with bifunctional active graphene skin and fast kinetics is well constructed to serve as the air cathode in metal-air batteries. Regulated oxygen species and three-dimensionally hierarchical porosity are well constructed on the carbon fiber surfaces, contributing high intrinsic activity and prominently enhanced kinetics, which leads to favorable performances in aqueous as well as flexible rechargeable zinc-air batteries. The work proposed a promising strategy in the rational design and smart synthesis of fast-kinetic monolith electrodes, which refreshes concepts and strategies of advanced material fabrication, and also bridges material science and practical energy devices.

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