Improving the sodium storage performance of carbonaceous anode: Synergistic coupling of pore structure and ordered domain engineering

The fundamental understanding on the relationship between the intrinsic textures and sodium storage performances of carbonaceous anodes is essential for the development of high-performance anodes for sodium-ion batteries (SIBs). However, the lack of methods to control the local atomic configurations of carbonaceous anodes has seriously hindered the revelation of the in-depth relationship between the designed structures and corresponding electrochemical performances. Herein, systematic measurements on the sodium storage of carbonaceous anodes derived from bimetallic-organic frameworks were reported with adjusted inner structure from hierarchical disordered structure to gradually increased graphitic ordered domains. Benefitting from the synergistic coupling of pore size controlling and ordered domain engineering, the optimized structure, featuring rich micropores/mesopores and ordered structure, possesses fast Na⁺ diffusion kinetics, low charge-transfer polarization, and favourable capacitive behaviors, thereby resulting in excellent sodium storage performances of 297.4 mAh g⁻¹ (0.1 A g⁻¹ up to 100 cycles) and 163.6 mAh g⁻¹ (1.0 A g⁻¹ up to 1000 cycles). Besides, this elaborate investigation might offer essential insights into the design of carbonaceous electrodes for efficient sodium storage.