Journal
CHEMICAL ENGINEERING JOURNAL
Volume 442, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.136258
Keywords
Defect engineering; Shuttling effect; Mn-N-C catalyst; Modified separators; Li-S batteries
Categories
Funding
- Science and Technology Innovation Fund of Dalian [2018J12GX052]
- National Natural Sci-ence Foundation of China [21776042, 21902021]
- Fundamental Research Funds for the Central Universities of China [DUT19ZD214]
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This study reports a defect engineering strategy using etch-evaporation to fabricate manganese-nitrogen doped porous carbon for separator modification. The modified separator exhibits high conductivity, strong immobilization and excellent catalytic activity, leading to improved performance of lithium-sulfur batteries.
Excellent specific discharge capacity and cycling stability are essential for high-performance lithium-sulfur (Li-S) batteries, but hard to achieve simultaneously due to the shuttle effect and sluggish reaction kinetics of poly-sulfides. Herein, we report an etch-evaporation enabled defect engineering strategy to fabricate atomically dispersed, manganese-nitrogen doped porous carbon (Mn-N-C) for separator modification. With Zinc atoms evaporation and NH3 etch, abundant spatial confinement sites and N dopants are created in Mn-N-C, and the final Mn loading can reach as high as 2.31 wt%. Density function theory (DFT) calculations reveal that Mn atoms in Mn-N-C play a crucial role in polysulfides adsorption and electrical conductivity enhancement. Therefore, the Mn-N-C modified separator can exhibit high conductivity, strong immobilization and excellent catalytic activity, thus favoring polysulfides conversion and Li2S nucleation/dissolution. The Li-S battery equipped with the modified separator exhibits an initial discharge capacity of 1596 mAh g(-1) at 0.1C (S loading mass was 1.2 mg cm-2), which decays 0.045 % per cycle after 1000 cycles at 1C. Our work demonstrates that the etch-evaporation enabled defect engineering strategy is effective for fabrication of high-performance Li-S battery catalyst; it also shows an attractive prospect to synthesize other high loading metal ion dispersed, nitrogen doped carbon materials for electrochemical applications.
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