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Heterostructure engineering for sulfur hosts is an effective way to achieve interfacial synergistic effects on suppressing the "shuttle effect" of polysulfides and thus improve electrochemical performance of lithium–sulfur (Li–S) batteries. Rational selection and design of different components into heterostructures is vital to enhance the synergistic effect. Herein, MoS2/MoP Mott–Schottky heterostructure nanoparticles decorated on reduced graphene oxide (MoS2/MoP@rGO) are fabricated and used as sulfur host firstly. Theoretical calculation and experiment results reveal that the in-situ introduction of MoP could tune the electronic structure, activate the basal plane of MoS2, and achieve the interfacial synergistic effects between adsorption (MoS2) and fast conversion (MoP). Such synergistic effects enable MoS2/MoP@rGO to not only remarkably facilitate Li2S deposition during the discharging process but also significantly accelerate the Li2S dissolution during the charging process, demonstrating bidirectional promotion behaviors. Thus, the designed cathode delivers initial capacity of 919.5 mA∙h∙g−1 with capacity of 502.3 mA∙h∙g−1 remaining after 700 cycles at 0.5 C. Even under higher sulfur loading of 4.31 mg∙cm−2 and lower electrolyte to sulfur (E/S) ratio of 8.21 μL∙mg−1, the MoS2/MoP@rGO@S cathode could still achieve good capacity and cycle stability. This work provides a novel and efficient structural design strategy of sulfur hosts for high-performance Li–S energy storage systems.


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Boosting bidirectional conversion of polysulfide driven by the built-in electric field of MoS2/MoP Mott–Schottky heterostructures in lithium–sulfur batteries

Show Author's information Meixiu Songa,bYanan Liua,b ( )Jingzhe Honga,bXiaoshuang Wanga,bXiaoxiao Huanga,b( )
School of Materials Science and Engineering, Harbin Institute of Technology, Harbin 150001, China
MIIT Key Laboratory of Advanced Structural–Functional Integration Materials & Green Manufacturing Technology, Harbin Institute of Technology, Harbin 150001, China

Abstract

Heterostructure engineering for sulfur hosts is an effective way to achieve interfacial synergistic effects on suppressing the "shuttle effect" of polysulfides and thus improve electrochemical performance of lithium–sulfur (Li–S) batteries. Rational selection and design of different components into heterostructures is vital to enhance the synergistic effect. Herein, MoS2/MoP Mott–Schottky heterostructure nanoparticles decorated on reduced graphene oxide (MoS2/MoP@rGO) are fabricated and used as sulfur host firstly. Theoretical calculation and experiment results reveal that the in-situ introduction of MoP could tune the electronic structure, activate the basal plane of MoS2, and achieve the interfacial synergistic effects between adsorption (MoS2) and fast conversion (MoP). Such synergistic effects enable MoS2/MoP@rGO to not only remarkably facilitate Li2S deposition during the discharging process but also significantly accelerate the Li2S dissolution during the charging process, demonstrating bidirectional promotion behaviors. Thus, the designed cathode delivers initial capacity of 919.5 mA∙h∙g−1 with capacity of 502.3 mA∙h∙g−1 remaining after 700 cycles at 0.5 C. Even under higher sulfur loading of 4.31 mg∙cm−2 and lower electrolyte to sulfur (E/S) ratio of 8.21 μL∙mg−1, the MoS2/MoP@rGO@S cathode could still achieve good capacity and cycle stability. This work provides a novel and efficient structural design strategy of sulfur hosts for high-performance Li–S energy storage systems.

Keywords: synergistic effect, shuttle effect, bidirectional polysulfide conversion, MoS2/MoP Mott–Schottky heterostructures, lithium–sulfur (Li–S) batteries

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Publication history

Received: 25 May 2023
Revised: 16 July 2023
Accepted: 02 August 2023
Published: 16 October 2023
Issue date: October 2023

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© The Author(s) 2023.

Acknowledgements

This work was supported by the National Natural Science Foundation of China (Grant Nos. 51772060, 51672059, 52372041, 52302087, and 51621091), Heilongjiang Touyan Team Program, and the Fundamental Research Funds for the Central Universities (Grant No.HIT. OCEF.2021003).

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