Hyperporous Sponge Interconnected by Hierarchical Carbon Nanotubes as a High‐Performance Potassium‐Ion Battery Anode

Recently, commercial graphite and other carbon‐based materials have shown promising properties as the anode for potassium‐ion batteries. A fundamental problem related to those carbon electrodes, significant volume expansion, and structural instability/collapsing caused by cyclic K‐ion intercalation, remains unsolved and severely limits further development and applications of K‐ion batteries. Here, a multiwalled hierarchical carbon nanotube (HCNT) is reported to address the issue, and a reversible specific capacity of 232 mAh g −1 , excellent rate capability, and cycling stability for 500 cycles are achieved. The key structure of the HCNTs consists of an inner CNT with dense‐stacked graphitic walls and a loose‐stacked outer CNT with more disordered walls, and individual HCNTs are further interconnected into a hyperporous bulk sponge with huge macropore volume, high conductivity, and tunable modulus. It is discovered that the inner dense‐CNT serves as a robust skeleton, and collectively, the outer loose‐CNT is beneficial for K‐ion accommodation; meanwhile the hyperporous sponge facilitates reaction kinetics and offers stable surface capacitive behavior. The hierarchical carbon nanotube structure has great potential in developing high‐performance and stable‐structure electrodes for next generation K and other metal‐ion batteries.