Asymmetric Configuration of Amorphous Mn-S Adjacent to Low-Nucleated MnS in N-Doped Carbon for Advanced Sodium-Ion Hybrid Capacitors #MMPMID41389034
Zhang K; He W; Zeng F; Huang Y; Wang T; Xie M; Ma D; Pan Y
Inorg Chem 2025[Dec]; ? (?): ? PMID41389034show ga
Addressing the kinetic mismatch and structural instability challenges in sodium-ion hybrid capacitor (SIHC) anodes, this study develops an N-doped carbon composite integrating amorphous Mn-S with adjacent low-nucleated MnS (a-Mn-S/MnS(LN)@NC). This architecture synergistically enhances mechanical stress buffering and charge transfer kinetics via the isotropic dynamic bonding of a-Mn-S and the high-affinity sites of MnS(LN). The 3D C-S-Mn covalent bonds in the a-Mn-S stabilize MnS(LN) through atomic anchoring, homogenizing volume strains and exposing uncoordinated S active sites to elevate Na(+) adsorption density. Theoretical calculations reveal that the proximity-induced d-p orbital hybridization reconstructs the electron-donor characteristics of S sites, creating an asymmetric electronic configuration. The electron-rich a-Mn-S serves as efficient Na(+) trapping centers, while the electron-deficient MnS(LN) facilitates rapid electron transfer. This configuration endows the composite with superior Na(+) adsorption energy and charge transfer efficiency over pure MnS. Consequently, the a-Mn-S/MnS(LN)@NC anode delivers a high reversible capacity of 597 mAh g(-1) at 0.1 A g(-1) and retains 90.5% capacity after 3500 cycles at 10.0 A g(-1). The assembled SIHCs achieve exceptional energy/power densities (186 Wh kg(-1) and 9576 W kg(-1)). This work elucidates the mechanism of adjacent asymmetric configurations for enhanced Na(+) storage, offering a novel strategy for designing high-performance SIHCs.
Inorg+Chem 2025 ; ? (?): ?
