Designing a better carbon framework is critical for harnessing the high theoretical capacity of Li-S batteries and avoiding their drawbacks, such as the insulating nature of sulfur, active material loss, and the polys...Designing a better carbon framework is critical for harnessing the high theoretical capacity of Li-S batteries and avoiding their drawbacks, such as the insulating nature of sulfur, active material loss, and the polysulfide shuttle reaction. Here, we report an ingenious design of hollow carbon nanofibers with closed ends and protogenetic mesopores in the shell that can be retracted to micropores after sulfur infusion. Such dynamic adjustable pore sizes ensure a high sulfur loading, and more importantly, eliminate excessive contact of sulfur species with the electrolyte. Together, the high aspect ratio and thin carbon shells of the carbon nanofibers facilitate rapid transport of Li^＋ ions and electrons, and the closed-end structure of the carbon nanofibers further blocks polysulfide dissolution from both ends, which is remarkably different from that for carbon nanotubes with open ends. The obtained sulfur-carbon cathodes exhibit excellent performance marked by high sulfur utilization, superior rate capability （1,170, 1,050, and 860 mA.h.g-1 at 1.0, 2.0, and 4.0 C （1 C = 1.675 A·g^-1）, respectively）, and a stable reversible capacity of 847 mA·h·g^-1 after 300 cycles at a high rate of 2.0 C.展开更多
基金This work was supported by the National Basic Research Program of China （No. 2013CB934104）, the National Natural Science Foundation of China （Nos. 21225312 and 21376047）, and Cheung Kong Scholars Program of China （No. T2015036）.
文摘Designing a better carbon framework is critical for harnessing the high theoretical capacity of Li-S batteries and avoiding their drawbacks, such as the insulating nature of sulfur, active material loss, and the polysulfide shuttle reaction. Here, we report an ingenious design of hollow carbon nanofibers with closed ends and protogenetic mesopores in the shell that can be retracted to micropores after sulfur infusion. Such dynamic adjustable pore sizes ensure a high sulfur loading, and more importantly, eliminate excessive contact of sulfur species with the electrolyte. Together, the high aspect ratio and thin carbon shells of the carbon nanofibers facilitate rapid transport of Li^＋ ions and electrons, and the closed-end structure of the carbon nanofibers further blocks polysulfide dissolution from both ends, which is remarkably different from that for carbon nanotubes with open ends. The obtained sulfur-carbon cathodes exhibit excellent performance marked by high sulfur utilization, superior rate capability （1,170, 1,050, and 860 mA.h.g-1 at 1.0, 2.0, and 4.0 C （1 C = 1.675 A·g^-1）, respectively）, and a stable reversible capacity of 847 mA·h·g^-1 after 300 cycles at a high rate of 2.0 C.
