.png){kind=icon}
.png){kind=icon}
Return
Orbital-engineered layered MnO2 cathode enabled by Ca2+ interlayer coupling in rechargeable calcium battery
.png){kind=icon}
PRE
AI
DOI：10.1016/j.jechem.2025.12.012.png)
.png){kind=icon}
Original request for help.png){kind=icon}
Share.png){kind=icon}
Save
Abstract
En 中文
Developing multivalent-ion storage systems demands cathode materials that combine high structural adaptability with favorable orbital interactions to host sluggish, highly charged carriers such as Ca2+. Herein, a multi-synergistic interlayer engineering strategy is proposed via Ca2+ interlayer coordination. The pre-coordination of Ca2+ ions establishes Mn–O–Ca bridges that not only expand the interlayer distance but also reshape the local orbital field of Mn, thereby stabilizing the high-valence Mn states and suppressing Jahn-Teller distortion. Defect-induced orbital reconfiguration simultaneously enhances electronic delocalization and interlayer polarity by creating localized charge imbalances at oxygen vacancies. As a result, efficient charge transfer and Ca2+ diffusion are promoted, and more surface-active sites are exposed. Electrochemical evaluations reveal that Ca-MnO2 exhibits significantly improved reversible capacity (∼100 mA h g−1 at 0.1 A g−1) and long-term cycling stability (1200 cycles at 1 A g−1), outperforming pristine δ-MnO2. Kinetic analysis through CV, GITT, and EIS demonstrates enhanced Ca2+ diffusion coefficients and reduced polarization in the pre-intercalated material. These results demonstrate an orbital-coupled interlayer engineering route toward high-performance Mn-based hosts for next-generation multivalent batteries.
Journal
IF:
14.9
Papers:
6.2K
Citations:
4.5W