Growing
attention has been attached to hard carbon in sodium-ion
batteries (SIBs). However, hard carbon from individual precursors
tends to exhibit an inferior rate capability due to its limited interlayer
distance. Here, a coupled strategy is designed to prepare hard carbon
microspheres (HCMSs) via the pyrolysis of a highly branched polymer
network formed instantaneously between two interactive precursors
during the atomization of the spray drying process. The combined precursors
with a tunable cross-linked structure prefer to generate a large interlayer
spacing (0.399 nm) and abundant closed pore structure by suppressing
the graphitization of precursors during the carbonization, relative
to the individual precursor, which contributes greatly to the ion
diffusion kinetics. Benefiting from the unique structure, HCMS exhibits
an impressively high reversible specific capacity of 373.4 mA h g–1 in SIBs and high initial Coulombic efficiency of
88%, retaining 90.2% of the initial capacity even after 150 cycles,
which presented comparable capacities with commercial graphite in
lithium-ion batteries. Besides, excellent rate capability was also
demonstrated with HCMSs (250 and 117 mA h g–1 at
300 and 600 mA g–1). Notably, the interlayer distance
and closed pore structure are tunable just by adjusting the ratio
of the two precursors. The tunable and extendable fabrication process,
together with its amazing high carbon yield of 48 wt % (1400 °C)
and high tap density close to 0.8 g cm–3, makes
this strategy promising in the practical application for SIBs.