4.6 Article

Competing reduction induced homogeneous oxygen doping to unlock MoS2 basal planes for faster polysulfides conversion

Journal

JOURNAL OF ENERGY CHEMISTRY
Volume 73, Issue -, Pages 26-34

Publisher

ELSEVIER
DOI: 10.1016/j.jechem.2022.06.002

Keywords

Competing reduction; One-pot; Oxygen-doped MoS2; Unlocked basal plane; Li-S batteries

Funding

  1. fund for Creative Research Groups of the National Natural Science Foundation of China [22021005]
  2. Science and Technology Innovation Fund of Dalian [2018J12GX052]
  3. National Natural Science Foundation of China [21776042, 22108027]
  4. Fundamental Research Funds for the Central Universities of China [DUT19ZD214]
  5. Shenzhen Science and Technology Program [201908163000519]
  6. GDSTC-Key R&D Project (GDSTC) [2019B090908001]

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This study presents a facile reduction strategy using ethylene glycol to dope oxygen atoms into MoS2, which unlocks its inert basal planes and enhances catalytic activity. The oxygen-doped MoS2 provides abundant adsorption/catalytic sites and improved ion transport, leading to improved performance of lithium sulfur batteries.
The parasitic polysulfides shuttle effect greatly hinders the practical application of lithium sulfur batteries, and this issue can be addressed by promoting polysulfides conversion with catalytic materials such as MoS2. However, the catalytic activity of MoS2 mainly relies on edge sites, but is limited by inert basal planes. We herein report a novel, facile, ethylene glycol enabled competing reduction strategy to dope MoS2 homogeneously with oxygen atoms so that its inert basal planes can be unlocked. Ethylene glycol works as a reducing agent and competes with thiourea to react with ammonium molybdate, leading to insufficient sulfuration of Mo, and consequent formation of O-MoS2. Our theoretical and experimental investigations indicate that the homogeneously distributed O dopants can create abundant adsorption/catalytic sites in the MoS2 basal planes, enlarge the inter-plane distance to promote ion transport, and thus enhance the catalytic conversion of polysulfides. The oxygen doped MoS2 (O-MoS2) is supported on carbon nanosheets (CNS) and the composite (O-MoS2/CNS) is employed to modify the separator of Li-S battery. It gives the battery an initial discharge capacity of 1537 mAh g(-1) at 0.2 C, and the battery retains a discharge capacity of 545 mAh g(-1) after ultra-long 2000 cycles at 1 degrees C, corresponding to a very small cyclic decay rate of 0.0237%. Even under a raising sulfur loading of 8.2 mg cm(-2), the Li-S battery also delivers a high discharge capacity (554 mAh g(-1)) with outstanding cycle stability (84.6% capacity retention) after 100 cycles at 0.5 degrees C. Our work provides a novel, facile approach to fabricate highly catalytically active oxygen-doped MoS2 for advanced Li-S batteries. (C) 2022 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved.

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