Energy, Environmental, and Catalysis Applications
- Zeru Wang
Zeru Wang
Shenzhen Key Laboratory of Intelligent Manufacturing for Continuous Carbon Fiber Reinforced Composites, Shenzhen 518055, P. R. China
School of System Design and Intelligent Manufacturing, Southern University of Science and Technology, Shenzhen 518055, P. R. China
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- Zhuang Xu
Zhuang Xu
Shenzhen Key Laboratory of Intelligent Manufacturing for Continuous Carbon Fiber Reinforced Composites, Shenzhen 518055, P. R. China
School of System Design and Intelligent Manufacturing, Southern University of Science and Technology, Shenzhen 518055, P. R. China
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- Yongbiao Mu
Yongbiao Mu
Department of Mechanical and Energy Engineering, Southern University of Science and Technology, Shenzhen 518055, P. R. China
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- Ben Slater
Ben Slater
Department of Chemistry, University of Oxford, Oxford OX1 2JD, U.K.
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- Jieyan Li
Jieyan Li
School of Science Shenzhen Key Laboratory of Flexible Printed Electronics Technology, Shenzhen Key Laboratory of Advanced Functional Carbon Materials Research and Comprehensive Application, Harbin Institute of Technology, Shenzhen 518055, P. R. China
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- Lin Zeng
Lin Zeng
School of Science Shenzhen Key Laboratory of Flexible Printed Electronics Technology, Shenzhen Key Laboratory of Advanced Functional Carbon Materials Research and Comprehensive Application, Harbin Institute of Technology, Shenzhen 518055, P. R. China
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- Ke Wang*
Ke Wang
Shenzhen Key Laboratory of Intelligent Manufacturing for Continuous Carbon Fiber Reinforced Composites, Shenzhen 518055, P. R. China
School of System Design and Intelligent Manufacturing, Southern University of Science and Technology, Shenzhen 518055, P. R. China
*Email: [emailprotected]
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ACS Applied Materials & Interfaces
Cite this: ACS Appl. Mater. Interfaces 2025, XXXX, XXX, XXX-XXX
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https://pubs.acs.org/doi/10.1021/acsami.4c22902
Published April 15, 2025
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Metal–organic frameworks (MOFs) show revolutionary potential in quasi-solid-state electrolytes (QSSEs) designed for high-energy-density batteries, owing to their tunable nanoporous structures and open metal sites (OMSs). However, their application is hindered by insufficient Li+ dissociation and low ionic conductivity, attributed to limited metal active sites. This study employed defect engineering to modulate hafnium-based MOFs, increasing OMS density while optimizing the pore microenvironment. The engineered defects improve the Lewis acid strength of OMSs, driving lithium salt dissociation and establishing strong chemisorption of TFSI– anions. By synergistically optimizing defect density, Lewis acidity, and structural stability, the defect-engineered Hf-MOF-QSSE achieved an ionic conductivity of 1.0 mS cm–1 at 30 °C and delivered a critical current density of 2 mA cm–2, surpassing previously reported MOF-QSSEs, underscoring the pivotal role of defect engineering in electrolyte optimization. Furthermore, Li||LiFePO4 cells exhibited excellent cycling stability and ultrahigh rate capability, retaining 93% of their capacity after 1500 cycles at 10C, while Li||NCM811 cells maintained a specific capacity of 85 mAh g–1 after 600 cycles at 5C.
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- Acidity
- Defects
- Electrolytes
- Lithium
- Metal organic frameworks
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ACS Applied Materials & Interfaces
Cite this: ACS Appl. Mater. Interfaces 2025, XXXX, XXX, XXX-XXX
Click to copy citationCitation copied!
Published April 15, 2025
Publication History
Received
Accepted
Revised
Published
online
© 2025 American Chemical Society
Request reuse permissions
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