Graphene Armored with a Crystal Carbon Shell for Ultrahigh-Performance Potassium Ion Batteries and Aluminum Batteries.

Graphene is of great significance in energy storage devices. However, a graphene-based electrode is difficult to use in direct applications due to the large surface area and flexibility, which leads to the excessive consumption of electrolyte, low Coulombic efficiency, and electrode shedding behaviors. Herein, a special crystal carbon@graphene microsphere (CCGM) composite was successfully synthesized. The scalable carbonaceous microsphere composite displays a small specific surface area and a superior structure stability. As a potassium ion battery electrode in a half-cell, CCGM delivers an initial capacity of 297.89 mAh g-1 with a high Coulombic efficiency of about 99%. It achieves an excellent cyclic stability with no capacity loss after 1250 cycles at the low current density of 100 mA g-1 with a long performing period of more than one year. As the cathode for an aluminum battery, a reversible specific capacity of 99.1 mAh g-1 at 1000 mA g-1 is obtained. CCGM delivers a long cycle performance of about 10 000 cycles at 4000 mA g-1 with a capacity retention of nearly 100%. Our design provides a fresh thought for the improvement of graphene-based materials, and it will greatly facilitate the application of graphene in the field of energy storage.