Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 8, Issue 23, Pages 14586-14595Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.6b03642
Keywords
hybrid separator; nitrogen/sulfur codoped; mesoporous carbon coating; polysulfide adsorption; DFT calculation; lithium-sulfur battery
Funding
- German Federal Ministry of Education and Research (BMBF) through the Excellent Battery-WING center Batteries - Mobility in Saxony [03X4637B, 03X4637C]
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Because of the outstanding high theoretical specific energy density of 2600 Wh kg(-1), the lithium-sulfur (Li-S) battery is regarded as a promising candidate for post lithium-ion battery systems eligible to meet the forthcoming market requirements. However, its commercialization on large scale is thwarted by fast capacity fading caused by the Achilles' heel of Li-S systems: the polysulfide shuttle. Here, we merge the physical features of carbon-coated separators and the unique chemical properties of N and S codoped mesoporous carbon to create a functional hybrid separator with superior polysulfide affinity and electrochemical benefits. DFT calculations revealed that carbon materials with N and S codoping possess a strong binding energy to high-order polysulfide species, which is essential to keep the active material in the cathode side. As a result of the synergistic effect of N, S dual-doping, an advanced Li-S cell with high specific capacity and ultralow capacity degradation of 0.041% per cycle is achieved. Pushing our simple-designed and scalable cathode to a highly increased sulfur loading of 5.4 mg cm(-2), the Li-S cell with the functional hybrid separator can deliver a remarkable areal capacity of 5.9 mAh cm(-2), which is highly favorable for practical applications.
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