▎ 摘　　要

Low-cost, high-performance oxygen catalysts are critical for electrochemical water splitting and metal-air bat-teries. Herein, carbon aerogels with skeletons consisting of few-layer graphene are derived pyrolytically from a hydrogel precursor using an array of NaCl crystals as the template, exhibiting a high electrical conductivity (869 S m-1) and an ultralow mass density (11.1 mg cm- 3). The deposition of NiFe layered double hydroxide (NiFe-LDH) nanocolloids renders the aerogels active towards both the oxygen reduction/evolution reactions (ORR/ OER), with the performances highly comparable to those of commercial benchmarks in both alkaline and neutral media. Results from operando Raman spectroscopy measurements and first principles caculations suggest that Fe (OH)3 colloids facilitate the oxidation of Ni2+, which lowers the energy barrier to 0.42 eV for OER, whereas the nitrogen-doped carbon aerogels are responsible for the ORR activity. With the composites used as bifunctional oxygen catalysts for electrochemical water splitting and rechargeable zinc-air batteries, the performances in both alkaline and neutral media are markedly better than those based on the mixture of commercial Pt/C and RuO2. Results from this study highlight the unique advantages of ultrathin graphene aerogels in the development of effective catalysts for electrochemical energy devices.