Abstract
Resins have shown significant potential as a precursor for hard carbons (HCs) in sodium-ion batteries (SIBs) due to their high purity and adjustability. However, the high cost and low Na+ storage capacity limit their industrialization. Herein, the highly crosslinked resin is developed by linear phenolic resin crosslinking with inexpensive hexamethylenetetramine (HMTA) via the C-N and methylene bridges between phenolic rings, which can effectively reduce the resin consumption ratio by over 44% per unit mass and regulate the sodium storage performance of the prepared HC with a high reversible capacity of 323.9 mAh g-1 and an initial coulombic efficiency (ICE) of 90.7% at 15 mA g−1, where a high plateau capacity of 286.8 mAh g-1 is proved to be a coupled storage mechanism of intercalation and pore-filling behavior. Meanwhile, defects associated with hydrogen content, rather than nitrogen defects, are verified to be directly linked to slope capacity. Furthermore, the 18650 cylindrical-type batteries assembled with this HC anode coupled with NaFe1/3Ni1/3Mn1/3O2 cathode achieve a high energy density of about 280.9 Wh kg−1 and excellent capacity retention of 86.4% over 2500 cycles, providing a promising prospect for the practical application of the resin-based HC for SIBs.
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