Exploration of Advanced Electrode Materials for Approaching High‐Performance Nickel‐Based Superbatteries

The surging interest in high performance, low‐cost, and safe energy storage devices has spurred tremendous research efforts in the development of advanced electrode active materials. Herein, the in situ growth of zinc–iron layered double hydroxide (Zn–Fe LDH) on graphene aerogel (GA) substrates through a facile, one‐pot hydrothermal method is reported. The strong interaction and efficient electronic coupling between LDH and graphene substantially improve interfacial charge transport properties of the resulting nanocomposite and provide more available redox active sites for faradaic reactions. An LDH–GA||Ni(OH)2 device is also fabricated that results in greatly enhanced specific capacity (187 mAh g−1 at 0.1 A g−1), outstanding specific energy (147 Wh kg−1), excellent specific power (16.7 kW kg−1), along with 88% capacity retention after >10 000 cycles. This approach is further extended to Ni–MH and Ni–Cd batteries to demonstrate the feasibility of compositing with graphene for boosting the energy storage performance of other well‐known Ni‐based batteries. In contrast to conventional Ni‐based batteries, the nearly flat voltage plateau followed by a sloping potential profile of the integrated supercapacitor–battery enables it to be discharged down to 0 V without being damaged. These findings provide new prospects for the design of high‐performance and affordable superbatteries based on earth‐abundant elements. An integrated superbattery device is demonstrated in which supercapacitive characteristics of a layered double hydroxide–graphene aerogel nanocomposite is effectively coupled with the battery‐like energy storage capacity of Ni(OH)2. This strategy offers new opportunities to improve high‐performance superbattery technologies that easily surpass conventional Ni‐based batteries and bring us a step closer to devices that possess the best characteristics of both supercapacitors and batteries.