Author(s) |
Thatsami, Niphat
Tangpakonsab, Parinya
Sikam, Pornsawan
Hussain, Tanveer
Tamwattana, Orapa
Watcharapasorn, Anucha
Moontragoon, Pairot
Pathak, Biswarup
Kaewmaraya, Thanayut
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Publication Date |
2024-07-24
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Abstract |
<p>The commercial viability of emerging lithium−sulfur batteries (LSBs) remains greatly hindered by short lifespans caused by electrically insulating sulfur, lithium polysulfides (Li<sub>2</sub>S<sub><i>n</i></sub>; 1 ≤ n ≤ 8) shuttling, and sluggish sulfur reduction reactions(SRRs). This work proposes the utilization of a hybrid composed of sulfiphilic MoS<sub>2</sub> and mayenite electride (C12A7:e<sup>−</sup>) as a cathode host to address these challenges. Specifically, abundant cement-based C12A7:e<sup>−</sup> is the most stable inorganic electrode, possessing the ultimate electrical conductivity and low work function. Through density functional theory simulations, the key aspects of the MoS<sub>2</sub>/C12A7:e<sup>−</sup> hybrid including electronic properties, interfacial binding with Li<sub>2</sub>S<sub><i>n</i></sub>, Li+ diffusion, and SRR have been unraveled. Our findings reveal the rational rules for MoS<sub>2</sub> as an efficient cathode host by enhancing its mutual electrical conductivity and surface polarity <i>via</i> MoS<sub>2</sub>/C12A7:e<sup>−</sup>. The improved electrical conductivity of MoS<sub>2</sub> is attributed to the electron donation from C12A7:e<sup>−</sup> to MoS<sub>2</sub>, yielding a semiconductor-to-metal transition. The resultant band positions of MoS<sub>2</sub>/C12A7:e<sup>−</sup> are well matched with those of conventional current-collecting materials (<i>i.e.</i>, Cu and Ni), electrochemically enhancing the electronic transport. Theaccepted charge also intensifies MoS<sub>2</sub> surface polarity for attracting polar Li<sub>2</sub>S<sub><i>n</i></sub> by forming stronger bonds with Li<sub>2</sub>S<sub><i>n</i></sub> <i>via</i> ionic Li−Sbonds than electrolytes with Li<sub>2</sub>S<sub><i>n</i></sub>, thereby preventing polysulfide shuttling. Importantly, MoS<sub>2</sub>/C12A7:e<sup>−</sup> not only promotes rapid reaction kinetics by reducing ionic diffusion barriers but also lowers the Gibbs free energies of the SRR for effective S<sub>8</sub>-to-Li<sub>2</sub>Sconversion. Beyond the reported applications of C12A7:e<sup>−</sup>, this work highlights its functionality as an electrode material to boost the efficiency of LSBs.</p>
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Citation |
ACS Applied Materials and Interfaces, 16(29), p. 37994-38005
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Link | |
Publisher |
American Chemical Society
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Rights |
Attribution-NonCommercial-NoDerivatives 4.0 International
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Title |
MoS2/Mayenite Electride Hybrid as a Cathode Host for Suppressing Polysulfide Shuttling and Promoting Kinetics in Lithium–Sulfur Batteries
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Type of document |
Journal Article
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Entity Type |
Publication
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Name | Size | format | Description | Link |
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openpublished/MoS2Hussain2024JournalArticle.pdf | 6584.374 KB | application/pdf | Published Version | View document |