Realizingthe Synergy of Interface and Dual-DefectEngineering for Molybdenum Disulfide Enables Efficient Sodium-IonStorage

Engineering-rich electrocatalyst defects play a critical role in greatly promoting the charge storage/transfer capability of an energy storage/conversion system. Here, an ingenious and effective two-step strategy was used to synthesize a bimetallic sulfide/oxide composite with a coaxial carbon coating, starting from mixing well-dispersed MoO<sub>3</sub> nanobelts and Co-PAA compound, followed by a selective etching process. The simultaneous formation of dual defects of interlayer defect and sulfur-rich vacancies as well as MoO<sub>2</sub>/MoS<sub>2‑<i>x</i></sub>/CoS heterojunctions noticeably enhances both electron transfer and ion diffusion kinetics. The ultrathin carbon protective layer on the surface of the composite ensures its high conductivity and excellent structural stability. The composite electrode shows a high reversible capacity (158.3 mAh g<sup>–1</sup> at 10 A g<sup>–1</sup> after 4000 cycles) and outstanding long-cycle stability (0.04% per cycle over 2100 cycles at 20 A g<sup>–1</sup>). A full cell based on MoO<sub>2</sub>/MoS<sub>2–<i>x</i></sub>/CoS@N, S–C anode, and Na<sub>3</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub> cathode can maintain a reversible capacity of 128.1 mAh g<sup>–1</sup> after 600 cycles at 1 A g<sup>–1</sup>, surpassing that based on MoO<sub>2</sub>/MoS<sub>2</sub> and is very comparable in performance with the state-of-the-art Na-ion full cells. Moreover, density functional theory (DFT) calculations, electrochemical kinetics analysis, and <i>in situ</i> Raman and <i>ex-situ</i> X-ray diffraction characterization were carried out to elucidate the involved scientific mechanisms of sodium storage.

Publication Details

Journal
Figshare
Published
2025-02-28
DOI
https://doi.org/10.1021/acsnano.4c17967.s001
Primary Topic
Electrocatalysts for Energy Conversion
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article
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Realizingthe Synergy of Interface and Dual-DefectEngineering for Molybdenum Disulfide Enables Efficient Sodium-IonStorage

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Electrocatalysts for Energy Conversion
article

Realizingthe Synergy of Interface and Dual-DefectEngineering for Molybdenum Disulfide Enables Efficient Sodium-IonStorage

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Abstract

Engineering-rich electrocatalyst defects play a critical role in greatly promoting the charge storage/transfer capability of an energy storage/conversion system. Here, an ingenious and effective two-step strategy was used to synthesize a bimetallic sulfide/oxide composite with a coaxial carbon coating, starting from mixing well-dispersed MoO<sub>3</sub> nanobelts and Co-PAA compound, followed by a selective etching process. The simultaneous formation of dual defects of interlayer defect and sulfur-rich vacancies as well as MoO<sub>2</sub>/MoS<sub>2‑<i>x</i></sub>/CoS heterojunctions noticeably enhances both electron transfer and ion diffusion kinetics. The ultrathin carbon protective layer on the surface of the composite ensures its high conductivity and excellent structural stability. The composite electrode shows a high reversible capacity (158.3 mAh g<sup>–1</sup> at 10 A g<sup>–1</sup> after 4000 cycles) and outstanding long-cycle stability (0.04% per cycle over 2100 cycles at 20 A g<sup>–1</sup>). A full cell based on MoO<sub>2</sub>/MoS<sub>2–<i>x</i></sub>/CoS@N, S–C anode, and Na<sub>3</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub> cathode can maintain a reversible capacity of 128.1 mAh g<sup>–1</sup> after 600 cycles at 1 A g<sup>–1</sup>, surpassing that based on MoO<sub>2</sub>/MoS<sub>2</sub> and is very comparable in performance with the state-of-the-art Na-ion full cells. Moreover, density functional theory (DFT) calculations, electrochemical kinetics analysis, and <i>in situ</i> Raman and <i>ex-situ</i> X-ray diffraction characterization were carried out to elucidate the involved scientific mechanisms of sodium storage.

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