Advancing high-temperature electrostatic energy storage via linker engineering of metal–organic frameworks in polymer nanocomposites

Zongliang Xie, Zhiyuan Huang, He Li, Tianlei Xu, Haoyu Zhao, Yunfei Wang, Xi Pang, Zhiqiang Cao, Virginia Altoé, Liana M. Klivansky, Zaiyu Wang, Steve W. Shelton, Shiqi Lai, Peng Liu, Chenhui Zhu, Michael D. Connolly, Corie Y. Ralston, Xiaodan Gu, Zongren Peng, Jian ZhangYi Liu

Research output: Contribution to journalArticlepeer-review

Abstract

High-performance, thermally resilient polymer dielectrics are essential for film capacitors used in advanced electronic devices and renewable energy systems, particularly at elevated temperatures where conventional polymers fail to perform. Compositing polymers with nanofillers is a well-established approach to enhancing energy storage performance, though there remains a strong need for fillers with broad structural tunability and a clear structure–property relationship to further improve performance at elevated temperatures. Herein, we unravel the untapped potential of UiO-66 metal–organic framework (MOF) derivatives as exceptional nanofillers for tuning the properties of the widely used polyetherimide (PEI). By systematically varying the linker structures, we create a series of isostructural MOF fillers that exhibit contrasting capabilities in regulating the charge transport and energy storage capacities of the resulting composite films. Notably, capacitors based on composite films using the electron-deficient UiO-66-F4 show remarkable long-term charge–discharge stability and achieve ultrahigh discharged energy densities of 9.87 J cm–3 at 150 1C and 9.21 J cm–3 at 200 1C, setting a new benchmark for high-temperature flexible polymer composites. Through comprehensive experimental and theoretical analyses, we establish an unprecedented correlation between the MOF fillers’ electronic structures and the composites’ improved electrical breakdown strength and energy storage properties. These findings offer a rational pathway to harness the exceptional structural diversity of MOFs for the development of composite materials suitable for high-temperature electrostatic energy storage.

Original languageEnglish
Pages (from-to)620-630
Number of pages11
JournalEnergy and Environmental Science
Volume18
Issue number2
DOIs
StatePublished - Nov 12 2024
Externally publishedYes

Funding

Z. X., H. L. and Y. L. acknowledge the support from the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division, under Contract no. DE-AC02-05CH11231 within the Inorganic/Organic Nanocomposites Program (KC3104). The synthesis and development of MOFs was supported by the Defense Threat Reduction Agency under award no. HDTRA241074. X. G. acknowledges the support from the U.S. Department of Energy, Office of Science, Office of Basic Energy Science under award no. DE-SC0022050. Work at the Molecular Foundry was supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract no. DE-AC02-05CH11231. This research used beamline 7.3.3 of the Advanced Light Source, which is a DOE Office of Science User Facility under contract no. DE-AC02-05CH11231. Y. W. was supported in part by an ALS Doctoral Fellowship in Residence. The authors thank Dr Antoine Lain\u00E9, Prof. Miquel Salmeron, Prof. Ting Xu, Dr Eric Dailing, Dr Zhen Xu, Dr Qingsong Zhang and Dr Lu Fan for discussions on experimental results, Haijuan Zhang and Dr Shihai Zhang for instrumental and technical support.

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