articleJournal of the American Chemical SocietyJan 9, 2026Closed access

Tailoring Lithium-Ion Coordination in Metal–Organic Frameworks via d-Orbital Control for Fast Ion Conduction

China University of Petroleum, East China · Division of Materials Science and Engineering · +2 more institutions

PubMed
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Abstract

The development of solid-state electrolytes (SSEs) is fundamentally constrained by the intrinsic trade-off between ionic transport efficiency and interfacial stability. While previous design strategies have enhanced lithium-ion conduction kinetics, the rational engineering of high-performance SSEs remains challenged by insufficient atomic-level insights into Li+ coordination microenvironments. Herein, we present a dynamic electronic-structure engineering approach utilizing π-conjugated two-dimensional metal–organic frameworks (M-4PyCN) with precisely modulated d-orbital occupation states. Through precision modulation of transition-metal centers, we achieve targeted charge density redistribution in cyanide…

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