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Title: Rational Design of a Dual-Function Hybrid Cathode Substrate for Lithium-Sulfur Batteries

Here, a unique 3D hybrid sponge with chemically coupled nickel disulfide–reduced graphene oxide (NiS 2–RGO) framework is rationally developed as an effective polysulfide reservoir through a biomolecule–assisted self–assembly synthesis. An optimized amount of NiS 2 (≈18 wt%) with porous nanoflower–like morphology is uniformly in situ grown on the RGO substrate, providing abundant active sites to adsorb and localize polysulfides. The improved polysulfide adsorptivity from sulfiphilic NiS 2 is confirmed by experimental data and first–principle calculations. Moreover, due to the chemical coupling between NiS 2 and RGO formed during the in situ synthesis, the conductive RGO substrate offers a 3D electron pathway to facilitate charge transfer toward the NiS 2–polysulfide adsorption interface, triggering a fast redox kinetics of polysulfide conversion and excellent rate performance (C/20–4C). Therefore, the self–assembled hybrid structure simultaneously promotes static polysulfide–trapping capability and dynamic polysulfide–conversion reversibility. As a result, the 3D porous sponge enables a high sulfur content (75 wt%) and a remarkably high sulfur loading (up to 21 mg cm –2) and areal capacity (up to 16 mAh cm –2), exceeding most of the reported values in the literature involving either RGO or metal sulfides/other metal compounds (sulfur content of <60 wt% and sulfur loading of <3more » mg cm –2).« less
Authors:
 [1] ;  [1] ; ORCiD logo [1]
  1. The Univ. of Texas at Austin, Austin TX (United States)
Publication Date:
Grant/Contract Number:
EE0007218
Type:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 8; Journal Issue: 24; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Research Org:
Univ. of Texas at Austin, Austin, TX (United States)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 25 ENERGY STORAGE; electrochemical performance; high‐loading cathodes; lithium–sulfur batteries; porous nanoflower‐like NiS2; reduced graphene oxide substrate
OSTI Identifier:
1487463
Alternate Identifier(s):
OSTI ID: 1456284

Luo, Liu, Chung, Sheng -Heng, and Manthiram, Arumugam. Rational Design of a Dual-Function Hybrid Cathode Substrate for Lithium-Sulfur Batteries. United States: N. p., Web. doi:10.1002/aenm.201801014.
Luo, Liu, Chung, Sheng -Heng, & Manthiram, Arumugam. Rational Design of a Dual-Function Hybrid Cathode Substrate for Lithium-Sulfur Batteries. United States. doi:10.1002/aenm.201801014.
Luo, Liu, Chung, Sheng -Heng, and Manthiram, Arumugam. 2018. "Rational Design of a Dual-Function Hybrid Cathode Substrate for Lithium-Sulfur Batteries". United States. doi:10.1002/aenm.201801014.
@article{osti_1487463,
title = {Rational Design of a Dual-Function Hybrid Cathode Substrate for Lithium-Sulfur Batteries},
author = {Luo, Liu and Chung, Sheng -Heng and Manthiram, Arumugam},
abstractNote = {Here, a unique 3D hybrid sponge with chemically coupled nickel disulfide–reduced graphene oxide (NiS2–RGO) framework is rationally developed as an effective polysulfide reservoir through a biomolecule–assisted self–assembly synthesis. An optimized amount of NiS2 (≈18 wt%) with porous nanoflower–like morphology is uniformly in situ grown on the RGO substrate, providing abundant active sites to adsorb and localize polysulfides. The improved polysulfide adsorptivity from sulfiphilic NiS2 is confirmed by experimental data and first–principle calculations. Moreover, due to the chemical coupling between NiS2 and RGO formed during the in situ synthesis, the conductive RGO substrate offers a 3D electron pathway to facilitate charge transfer toward the NiS2–polysulfide adsorption interface, triggering a fast redox kinetics of polysulfide conversion and excellent rate performance (C/20–4C). Therefore, the self–assembled hybrid structure simultaneously promotes static polysulfide–trapping capability and dynamic polysulfide–conversion reversibility. As a result, the 3D porous sponge enables a high sulfur content (75 wt%) and a remarkably high sulfur loading (up to 21 mg cm–2) and areal capacity (up to 16 mAh cm–2), exceeding most of the reported values in the literature involving either RGO or metal sulfides/other metal compounds (sulfur content of <60 wt% and sulfur loading of <3 mg cm–2).},
doi = {10.1002/aenm.201801014},
journal = {Advanced Energy Materials},
number = 24,
volume = 8,
place = {United States},
year = {2018},
month = {6}
}

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