Covalently Integrated Amorphous Mn x Mo 3 S 13 –GO Chalcocarbogel for High Capacity and Long‐Life Sulfur Equivalent Conversion Electrodes

Résumé fourni par la source

ABSTRACT Developing long‐life, high‐capacity sulfur‐based electrodes from earth‐abundant elements remains a major challenge because of structural degradation and polysulfide dissolution during multielectron conversion reactions. Here, we report a hybrid amorphous Mn x Mo 3 S 13 –GO (x = 0.5) chalcocarbogel synthesized by a room‐temperature, acid‐free sol–gel process. The resulting framework comprises chemically integrated M─S/O, (M = Mn, Mo), and C─S bonding motifs that form a mechanically and chemically robust electroactive network. Synchrotron X‐ray PDF, XANES/EXAFS, XPS, Raman spectroscopy, magnetic susceptibility, and density functional theory (DFT)‐based ab initio molecular dynamics reveal short‐range Mo 3 S 13 ‐like clusters and MnS 2 ‐like coordination environments within the amorphous framework. Mn incorporation shortens polysulfide chains and strengthens Lewis acid–base interactions with redox‐active sulfur species, while graphene oxide enhances electronic connectivity and structural integrity through chemically coupled interfaces. As a lithium‐ion battery cathode, the Mn x Mo 3 S 13 –GO chalcocarbogel delivers a reversible capacity of ∼525 mAh g − 1 after 1000 cycles at C/3, corresponding to 83% capacity retention with >99.99% Coulombic efficiency. These findings establish Mo 3 S 13 cluster‐engineered chalcocarbogels as a versatile platform for durable amorphous sulfur‐redox electrodes, where synergistic metal–sulfur and graphene oxide interactions at the atomic level enable long‐term electrochemical stability and high‐performance energy storage.

Ce résumé expose les affirmations des auteurs. BNTIC ne l’interprète pas comme une validation indépendante des résultats.