Qian Yu, Xiaojun Shi, Taoqiu Zhang, Yi Zhao, Jun Jin, Rui Wang, Yansheng Gong, Huanwen Wang
Extremely fast-charging and long-life span are critical yet challenging for the development of cost-effective and sustainable potassium-ion batteries (PIBs) due to the sluggish kinetics and rapid capacity decay of graphite anodes caused by the large radius of K ions (1.38 Å). To tackle this issue, here a new type of nitrogen-doped graphitic carbon tubes (NGCTs) is reported via a ZrO2-templated chemical vapor deposition (CVD) approach. The carbon interlayer spacing, crystallite size, and N-configurations in NGCTs are controlled by adjusting the CVD temperature (800, 900, 1000 °C). The optimized NGCT-900 sample well balances the graphitic domains and structural defects, thus enabling fast K+ insertion/extraction below 1 V (vs. K+/K). These tubular carbon membranes achieve exceptional K+-storage performance including high K+-storage capacities of 404 mAh g−1 at 0.1 A g−1, ultrafast charging at 50 A g−1 and a super-long cycle life of up to 6,000 cycles. Ex-situ XRD, in-situ Raman, and GITT analyses reveal a synergistic K+-adsorption-intercalation mechanism. Further comparison with S or P heteroatoms underscores the significance of N-doping in enhancing reversible K+ intercalation into graphitic domains and boosting surface adsorption capacity. The fabricated NGCT-900//KxNi0.33Mn0.67O2 PIB (1.2~3.2 V) provides both a high-energy density of 187 Wh kg−1 (comparable to graphite//LiFePO4 LIBs) and a high-power density of 2200 W kg−1 at 123 Wh kg−1. This study establishes a carbon anode design strategy for advanced potassium storage.