journal article·2026-04

Polarization Regulation of Alkali‐Treated Metal–Organic Frameworks for Dual‐Functional Dielectrics

Song Ye, Seemab Hussnain, Kang Wang, Jiajun Yu, Lai Jiang, Juan Liu, Aming Xie, Wai‐yeung Wong, Roland A. Fischer, Soumya Mukherjee, Weijin Li, Haibo Zeng

Advanced Functional Materials· Volume 36· Issue 35
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Abstract

ABSTRACT Coordination bond breakage and rearrangement offer a previously unexplored route to enhance the dielectric properties of metal–organic frameworks (MOFs). Here, we introduce a controlled alkali‐treatment strategy to regulate polarization and energy storage in 2D M‐TA MOFs (M = Ni, Co, NiCo; TA = terephthalate). Hydrolysis of metal nodes by OH − generates ionic species and is thus prone to forming to architectures that amplify polarization. Co‐TA derivatives treated for 16 min exhibit a dielectric constant of ε ≈ 27.8, ca. 4×higher than the pristine framework, while Ni‐TA and NiCo‐TA reveal improvements owing to stronger metal–ligand coupling. Thin films of NiCo‐TA‐2 display ultralow leakage currents (< 10 −11 A·cm −2 ) and robust mechanical performance (Young's modulus ≈ 0.92 GPa), highlighting their promise as high‐κ gate dielectrics. When integrated into PVDF composites, treated MOFs deliver energy storage densities up to 2.74 J·cm −3 , comparable to leading non‐ferroelectric polymers. (Biaxially oriented polypropylene, a general commercial dielectric film, whose energy storage density down to 0.3 J·cm −3 and 5 MV/cm). These findings establish coordination‐bond rearrangement as a powerful design principle for dielectric optimization in MOFs, offering a route to mitigate polarization–conductivity trade‐offs and expand their applicability in advanced electronic and energy‐storage technologies.
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Research context

OpenAlex topics: Dielectric materials and actuators · Dielectric properties of ceramics · Advanced Sensor and Energy Harvesting Materials

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Affiliations

MIIT Key Laboratory of Advanced Display Materials and Devices & Materials Physical and Chemical Research and Practice Center College of Materials Science and Engineering Nanjing University of Science and Technology Nanjing P. R. China

State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou P. R. China

School of Chemistry and Life Sciences Nanjing University of Posts and Telecommunications Nanjing P. R. China

School of Safety Science and Engineering Nanjing University of Science and Technology Nanjing P. R. China

Department of Applied Biology and Chemical Technology and Research Institute for Smart Energy The Hong Kong Polytechnic University Hong Kong Hung Hom P. R. China

Chair of Inorganic and Metal‐Organic Chemistry Department of Chemistry & Catalysis Research Center School of Natural Sciences Technical University of Munich Garching Germany

Department of Chemical Sciences Bernal Institute and Research Ireland Centre for Pharmaceuticals (SSPC) University of Limerick Limerick Ireland

Funding

National Natural Science Foundation of China · Fundamental Research Funds for the Central Universities

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