Journal
ENERGY & ENVIRONMENTAL SCIENCE
Volume 12, Issue 10, Pages 2976-2982Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c9ee01257e
Keywords
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Funding
- National Key Research and Development Program [2016YFA0202500, 2016YFA0200102]
- National Natural Science Foundation of China [21676160, 21776019, 21825501, 21805162, U1801257]
- China Postdoctoral Science Foundation [2018M630165]
- Beijing Key Research and Development Plan [Z181100004518001]
- Tsinghua University Initiative Scientific Research Program
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Lithium-sulfur (Li-S) batteries with a high theoretical energy density basedonmulti-electron redox reactionswere strongly considered. The lithium disulfide/sulfide (Li2S2/Li2S, denoted as Li2S1/2) precipitation is critical to achieve high sulfur utilization. However, the kinetic effect on Li2S1/2 precipitation in a working battery has been rarely investigated. Herein, the current-density-dependent Li2S1/2 nucleation/growth was explored and such a dependence served as the guiding principle for the construction of high-sulfur-loading/content Li-S batteries. Generally, the Li2S1/2 nucleation density is proportional to two-third the power of the current density and the shift from a high to low current density alters the Li2S1/2 precipitation pathway from surface deposition to solution-mediated growth. The in-solution growth rate was found to be restricted by the mobilities of polysulfide intermediates and Li2S1/2 in conventional ether electrolytes. The rationalized guideline directed the design of a lightweight, high-surface-area, and open-pore conductive framework for sulfur cathodes, which enabled an extremely high sulfur content of 93.4 wt% in the whole electrode and a high capacity (1269 mA h g(-1)). The present work affords a kinetic understanding of the liquid-solid conversion in working Li-S batteries and optimization schemes for practical operation parameters.
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