Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 37, Pages 20286-20293Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202108317
Keywords
aqueous Zn-ion batteries; cathode materials; DFT computations; molecular engineering; MoS2
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Funding
- National Natural Science Foundation of China [21805007, 22075016]
- Beijing Natural Science Foundation [L182019]
- Fundamental Research Funds for the Central Universities [FRF-TP-20-020A3, FRF-TP-18-091A1]
- 111 Project [B12015, B170003]
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The study introduces a molecular engineering strategy for MoS2 cathodes, involving the manufacturing of structure defects and O-doping to unlock the inactive basal plane and increase the interlayer spacing, leading to the production of abundant 1T-phase for enhanced Zn2+ transport. The tailored D-MoS2-O material exhibits excellent hydrophilicity and high conductivity, allowing for high-rate capability and stable performance in a wearable rechargeable Zn battery, showcasing great application potential for aqueous Zn-ion batteries.
Aqueous Zn-storage behaviors of MoS2-based cathodes mainly rely on the ion-(de)intercalation at edge sites but are limited by the inactive basal plane. Herein, an in-situ molecular engineering strategy in terms of structure defects manufacturing and O-doping is proposed for MoS2 (designated as D-MoS2-O) to unlock the inert basal plane, expand the interlayer spacing (from 6.2 to 9.6 angstrom), and produce abundant 1T-phase. The tailored D-MoS2-O with excellent hydrophilicity and high conductivity allows the 3D Zn2+ transport along both the ab plane and c-axis, thus achieving the exceptional high rate capability. Zn2+ diffusion through the basal plane is verified by DFT computations. As a proof of concept, the wearable quasi-solid-state rechargeable Zn battery employing the D-MoS2-O cathode operates stably even under severe bending conditions, showing great application prospects. This work opens a new window for designing high-performance layered cathode materials for aqueous Zn-ion batteries.
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