▎ 摘　　要

Currently, the low energy efficiency of water electrolysis has compelled research toward the development of novel and energy-effective strategies for low-cost H-2 generation. In this context, we report a new concept of simultaneous H-2 and electricity generation by separating out the exothermic self-sustained Al-H2O reaction via electrochemistry. In addition, to catalyze the cathodic water reduction reaction, a single-pot and environmentally benign synthesis method is adopted. It results in the design of an electrocatalyst composed of Co@CoAl-layered double hydroxide core-shell nanospheres anchored over in situ generated N-doped graphene. Toward the water reduction reaction, the designed catalyst shows a negative voltage shift of mere around 113 mV with respect to the commercial Pt/C catalyst to reach the benchmark 10 mA cm(-2), with excellent stability of approximately 86 % voltage retention after 12 h of continuous operation. The catalytic superiority of our material is evident when taken for battery-level testing; the fabricated device was able to deliver an average output voltage of around 0.95 V at a discharge current density of 5 mA cm(-2) along with H-2 liberation, which was also detected and quantified through gas chromatography.