TY - JOUR
T1 - Suppressed polysulfide crossover in Li−S batteries through a high-flux graphene oxide membrane supported on a sulfur cathode
AU - Shaibani, Mahdokht
AU - Akbari, Abozar
AU - Sheath, Phillip Andrew
AU - Easton, Christopher D.
AU - Chakraborty Banerjee, Parama
AU - Konstas, Kristina
AU - Fakhfouri, Armaghan
AU - Barghamadi, Marzieh
AU - Musameh, Mustafa M.
AU - Best, Adam S.
AU - Ruther, Thomas
AU - Mahon, Peter J.
AU - Hill, Matthew R.
AU - Hollenkamp, Anthony F.
AU - Majumder, Mainak
PY - 2016/7/11
Y1 - 2016/7/11
N2 - Utilization of permselective membranes holds tremen-dous promise for retention of the electrode-active material in electrochemical devices that suffer from electrode instability issues. In a rechargeable Li−S battery--a strong contender to outperform the Li-ion technologymigration of lithium polysulfides from the sulfur cathode has been linked to rapid capacity fading and lower Coulombic efficiency. However, the current approaches for configuring Li−S cells with permselective membranes suffer from large ohmic polarization, resulting in low capacity and poor rate capability. To overcome these issues, we report the facile fabrication of a high-flux graphene oxide membrane directly onto the sulfur cathode by shear alignment of discotic nematic liquid crystals of graphene oxide (GO). In conjunction with a carbon-coated separator, the highly ordered structure of the thin (∼0.75 µm) membrane and its inherent surface charge retain a majority of the polysulfides, enabling the cells to deliver very high initial discharge capacities of 1063 and 1182 mAh g-1electrode for electrodes with 70 and 80% sulfur content, respectively, at the practical 0.5 C rate. The very high sulfur utilization and impressive capacity retentions of the high sulfur content electrodes result in some of the highest performance metrics in the literature of Li−S (e.g., electrode capacity of 835 mAh g-1electrode after 100 cycles at 0.5 C with a sulfur content of 80%). We show that the structural order of the shear-aligned GO membrane is key in maintaining good kinetics of the charge transfer processes in Li-S batteries.
AB - Utilization of permselective membranes holds tremen-dous promise for retention of the electrode-active material in electrochemical devices that suffer from electrode instability issues. In a rechargeable Li−S battery--a strong contender to outperform the Li-ion technologymigration of lithium polysulfides from the sulfur cathode has been linked to rapid capacity fading and lower Coulombic efficiency. However, the current approaches for configuring Li−S cells with permselective membranes suffer from large ohmic polarization, resulting in low capacity and poor rate capability. To overcome these issues, we report the facile fabrication of a high-flux graphene oxide membrane directly onto the sulfur cathode by shear alignment of discotic nematic liquid crystals of graphene oxide (GO). In conjunction with a carbon-coated separator, the highly ordered structure of the thin (∼0.75 µm) membrane and its inherent surface charge retain a majority of the polysulfides, enabling the cells to deliver very high initial discharge capacities of 1063 and 1182 mAh g-1electrode for electrodes with 70 and 80% sulfur content, respectively, at the practical 0.5 C rate. The very high sulfur utilization and impressive capacity retentions of the high sulfur content electrodes result in some of the highest performance metrics in the literature of Li−S (e.g., electrode capacity of 835 mAh g-1electrode after 100 cycles at 0.5 C with a sulfur content of 80%). We show that the structural order of the shear-aligned GO membrane is key in maintaining good kinetics of the charge transfer processes in Li-S batteries.
U2 - 10.1021/acsnano.6b03285
DO - 10.1021/acsnano.6b03285
M3 - Article
VL - 10
SP - 7768
EP - 7779
JO - ACS Nano
JF - ACS Nano
SN - 1936-0851
IS - 8
ER -