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Vol. 18 (2026)

Confining Li⁺ Solvation in Core–Shell Metal–Organic Frameworks for Stable Lithium Metal Batteries at 100 °C

https://doi.org/10.1007/s40820-025-01988-7
Minh Hai Nguyen
Department of Materials Science and Engineering, Chungnam National University, Daejeon 34134, Republic of Korea
Jeongmin Shin
School of Mechanical Engineering, Chonnam National University, Gwangju 61186, Republic of Korea
Mee‑Ree Kim
Department of Materials Science and Engineering, Chungnam National University, Daejeon 34134, Republic of Korea
Quan Van Nguyen
Department of Materials Science and Engineering, Chungnam National University, Daejeon 34134, Republic of Korea
JinHyeok Cha
School of Mechanical Engineering, Chonnam National University, Gwangju 61186, Republic of Korea
Sangbaek Park
Department of Materials Science and Engineering, Chungnam National University, Daejeon 34134, Republic of Korea

Corresponding Author: Sangbaek Park

sb.park@cnu.ac.kr

Nano-Micro Letters, Vol. 18 (2026), Article Number: 135

Abstract

The practical deployment of lithium metal batteries remains severely constrained, especially under elevated temperatures. Although metal–organic frameworks (MOFs) improve the thermal stability of liquid electrolytes by capturing them in well-ordered sub-nanopores, interparticle voids between MOF particles readily absorb liquid electrolyte, obscuring our understanding of the intrinsic role of nanopores in directing Li⁺ transport. To address this challenge, we introduce a one-dimensional (1D) MOF model architecture that eliminates interparticle effects and enables direct observation of Li⁺ solvation and de-solvation dynamics. Comparative studies of 1D HKUST-1 and ZIF-8 uncover distinct transport behaviors, supported by both experimental measurements and neural network potential-based molecular dynamics simulations. Building on these insights, we construct a hierarchical core–shell MOF architecture by integrating ZIF-8 (core) and HKUST-1 (shell) onto a hybrid fiber scaffold. This design harnesses the complementary strengths of both MOFs to achieve continuous ion pathways, directional Li⁺ conduction, and improved thermal and electrochemical resilience.


Highlights:
1 We report the in-situ growth of core–shell metal-organic frameworks on glass fiber, creating a binder-free quasi-solid-state electrolytes (QSSEs) with multiple Li+ transport pathways.
2 Pore-size-dependent solvation and de-solvation structures of Li+ are confined within HKUST-1 and ZIF-8 channels, enabling tailored ion dynamics.
3 The core–shell QSSE achieves high Li+ conductivity, suppressed dendrite growth, and stable Li plating/stripping under high-temperature conditions.
4 Lithium metal batteries with the core–shell QSSE show exceptional cycling stability at 100 °C.

Keywords

Quasi-solid-state electrolyte Metal–organic frameworks Li metal batteries Thermal stability Lithium-ion solvation/de-solvation
Nguyen, Minh Hai, Jeongmin Shin, Mee‑Ree Kim, Quan Van Nguyen, JinHyeok Cha, and Sangbaek Park. 2026. “Confining Li⁺ Solvation in Core–Shell Metal–Organic Frameworks for Stable Lithium Metal Batteries at 100 °C”. Nano-Micro Letters 18 (January):135. https://doi.org/10.1007/s40820-025-01988-7.
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