Strengthened d-p Orbital Hybridization on Metastable Cubic Mo 2 C for Highly Stable Lithium-Sulfur Batteries.

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  • Additional Information
    • Source:
      Publisher: American Chemical Society Country of Publication: United States NLM ID: 101313589 Publication Model: Print-Electronic Cited Medium: Internet ISSN: 1936-086X (Electronic) Linking ISSN: 19360851 NLM ISO Abbreviation: ACS Nano Subsets: PubMed not MEDLINE; MEDLINE
    • Publication Information:
      Original Publication: Washington D.C. : American Chemical Society
    • Abstract:
      Suppressing the lithium polysulfide (LiPS) shuttling as well as accelerating the conversion kinetics is extremely crucial yet challenging in designing sulfur hosts for lithium-sulfur (Li-S) batteries. Phase engineering of nanomaterials is an intriguing approach for tuning the electronic structure toward regulating phase-dependent physicochemical properties. In this study, a metastable phase δ-Mo 2 C catalyst was elaborately synthesized via a boron doping strategy, which exhibited a phase transfer from hexagonal to cubic structure. The hierarchical tubular structure of the metastable cubic δ-Mo 2 C-decorated N-doped carbon nanotube (δ-B-Mo 2 C/NCNT) endows fast electron transfer and abundant polar sites for LiPSs. First-principles calculations reveal the strengthened chemical adsorption capability and hybridization between the d orbital of Mo metal and the p orbital of S atoms in LiPSs, contributing to higher electrocatalytic activity. Moreover, in situ Raman analysis manifests accelerated redox conversion kinetics. Consequently, δ-B-Mo 2 C/NCNT renders the Li-S battery with a high specific capacity of 1385.6 mAh g -1 at 0.1 C and a superior rate property of 606.3 mAh g -1 at 4 C. Impressively, a satisfactory areal capacity of 6.95 mAh cm -2 is achieved under the high sulfur loading of 6.8 mg cm -2 . This work has gained crucial research significance for metastable catalyst design and phase engineering for Li-S batteries.
    • Contributed Indexing:
      Keywords: Mo2C; lithium−sulfur batteries; metastable electrocatalysts; orbital hybridization; polysulfide conversion
    • Publication Date:
      Date Created: 20241213 Latest Revision: 20241224
    • Publication Date:
      20241224
    • Accession Number:
      10.1021/acsnano.4c11701
    • Accession Number:
      39668735