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Interlayer Spacing Control of MoS2 with Covalent Thiol Functionalization: Understanding Structure and
Jaehoon Choi1,2, Kyeonghyeon Nam3, Yoga T Malik1,2
1Helmholtz Institute Ulm (HIU), Helmholtzstraße 11, 89081 Ulm, Germany.
Covalent functionalization of molybdenum disulfide (MoS2) with dithiols expands interlayer spacing for enhanced lithium-ion storage. However, optimal performance requires careful control of dithiol loading to balance capacity and ion transport.
Area of Science:
- Materials Science
- Electrochemistry
- Nanotechnology
Background:
- Molybdenum disulfide (MoS2) is a promising 2D material for energy storage.
- Increasing interlayer spacing in MoS2 enhances ion intercalation capacity and kinetics.
- Controlling interlayer spacing is crucial for optimizing MoS2-based electrode performance.
Purpose of the Study:
- To explore covalent thiol functionalization for controlling MoS2 interlayer spacing.
- To investigate the influence of dithiol pillar loading on MoS2 structure and electrochemistry.
- To understand the structure-property relationships in functionalized MoS2 for energy storage.
Main Methods:
- Hydrothermal bottom-up synthesis to incorporate dithiolated molecules into the MoS2 lattice.
- Comprehensive experimental characterization (e.g., structural analysis, electrochemical testing).
- Computational simulations to analyze pillar-host interactions and Li+ transport.
Main Results:
- Dithiol incorporation leads to interlayer expansion, increasing Li+ storage capacity (max 1.43 Li+/MoS2).
- Low dithiol loading results in pillar clustering and inhomogeneous expansion.
- High dithiol loading causes defective bonding and impedes Li+ transport, negatively impacting performance.
Conclusions:
- Covalent dithiol functionalization offers a route to tune MoS2 interlayer spacing for energy storage.
- Optimizing dithiol density is critical to maximize capacity while maintaining efficient ion transport.
- Findings provide insights for designing advanced transition metal dichalcogenide electrode materials.
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