Studies on electrochemical sodium storage into hard carbons with binder-free monolithic electrodes

• Electrochemical Na+-storage in hard carbons is explored using monolithic electrodes.
• The Na+-insertion behaviors into hard carbons calcined at 800–3000 °C are compared.
• The difference between Li+ and Na+ ion-trapping in nanovoids is demonstrated.
• The effect of pore size on the initial irreversible capacity is discussed.

Hard carbons emerge as one of the most promising candidate for an anode of Na-ion batteries. This research focuses on the carbon monolith derived from resorcinol-formaldehyde (RF) gels as a model hard carbon electrode. A series of binder-free monolithic carbon electrodes heat-treated at varied temperatures allow the comparative investigation of the correlation between carbon nanotexture and electrochemical Na+-ion storage. The increase in carbonization temperature exerts a favorable influence on electrode performance, especially in the range between 1600 °C and 2500 °C. The comparison between Li+- and Na+-storage behaviors in the carbon electrodes discloses that the Na+-trapping in nanovoids is negligible when the carbonization temperature is higher than 1600 °C. On the other hand, the high-temperature sintering at 2500–3000 °C enlarges the resistance for Na+-insertion into interlayer spacing as well as Na+-filling into nanovoids. In addition, the study on the effect of pore size clearly demonstrates that not the BET surface area but the surface area related to meso- and macropores is a predominant factor for the initial irreversible capacity. The outcomes of this work are expected to become a benchmark for other hard carbon electrodes prepared from various precursors.

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