In this study, we aimed to demonstrate the effects of the structure and dopants of the carbon framework on the electrochemical performances of the Se-S/C cathode. We prepared the SeS2/C composites by a facile melt-diffusion and an evaporation method employing 4 different carbon frameworks; (i) mesoporous carbon(OMC), (ii) nitrogen-doped ordered mesoporous carbon(NOMC), (iii) sulfur-doped ordered mesoporous carbon(SOMC), and (iv) ketjen black 600JD (KB600, commercial carbon). When preparing the SeS2/C composites, we intended that the SeS2 was partially filled on the carbon frameworks by making an inside hole of SeS2 inside pores of carbon framework, as shown in Fig. 1-2. We believed that it would be beneficial to suppressing volume expansion of chalcogen materials and utilization of the active materials.
From the half-cell tests of four SeS2/C cathodes (SeS2/OMC, SeS2/NOMC, SeS2/SOMC, and SeS2/KB600) (Fig.3), the SeS2/KB600 showed the highest initial capacity due to its largest surface area that provides sufficient electrochemical reaction sites. However, it exhibited a poor cyclic stability due to the continuous dissolution of lithium polysulfides and polyselenides, originated from relatively large mean pore diameter (8.67 nm >) that is not suitable to trap the Se and S physically. Meanwhile, the SeS2 in the 3 types of ordered mesoporous carbons (OMC, NOMC, and SOMC), which have a large length to pore diameter ratio (L/D), delivered better rate-capability than the spherical KB600 (Fig. 3a). It implies that a long diffusion path for Li ions and partially filled SeS2 in the ordered mesoporous carbons are favorable to ion transportation inside pores [4]. Among all the SeS2/C cathodes, SeS2/NOMC exhibited the best electrochemical performance; nearly 99.99 % coulombic efficiency (no capacity fading during 500 cycles) presumably due to its N dopant that contribute to chemical adsorption of the soluble intermediates (Fig. 3b, 4).
References
[1] K. Eom et al., Nature communications 8 (2017) 13888
[2] Z. Li et al., Adv. Energy Mater (2017) 170028
[3] Sun et al., ACS Nano 6 (2016) 8289-8298