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Largely Pseudocapacitive Two-Dimensional Conjugated Metal–Organic Framework Anodes with Lowest Unoccupied Molecular Orbital Localized in Nickel-bis(dithiolene) Linkages

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    Largely Pseudocapacitive Two-Dimensional Conjugated Metal–Organic Framework Anodes with Lowest Unoccupied Molecular Orbital Localized in Nickel-bis(dithiolene) Linkages
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    • Panpan Zhang
      Panpan Zhang
      State Key Laboratory of Materials Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, 430074 Wuhan, China
      Center for Advancing Electronics Dresden (cfaed) and Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Mommsenstr. 4, 01062 Dresden, Germany
      More by Panpan Zhang
      Orcidhttps://orcid.org/0000-0002-3967-6548
    • Mingchao Wang*
      Mingchao Wang
      Center for Advancing Electronics Dresden (cfaed) and Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Mommsenstr. 4, 01062 Dresden, Germany
      *Email: [email protected]
      More by Mingchao Wang
      Orcidhttps://orcid.org/0000-0001-9979-3503
    • Yannan Liu
      Yannan Liu
      Center for Advancing Electronics Dresden (cfaed) and Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Mommsenstr. 4, 01062 Dresden, Germany
      Max Planck Institute of Microstructure Physics, D-06120 Halle (Saale), Germany
      More by Yannan Liu
      Orcidhttps://orcid.org/0000-0002-7379-3385
    • Yubin Fu
      Yubin Fu
      Center for Advancing Electronics Dresden (cfaed) and Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Mommsenstr. 4, 01062 Dresden, Germany
      Max Planck Institute of Microstructure Physics, D-06120 Halle (Saale), Germany
      More by Yubin Fu
      Orcidhttps://orcid.org/0000-0002-2613-394X
    • Mingming Gao
      Mingming Gao
      State Key Laboratory of Materials Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, 430074 Wuhan, China
      More by Mingming Gao
    • Gang Wang
      Gang Wang
      Center for Advancing Electronics Dresden (cfaed) and Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Mommsenstr. 4, 01062 Dresden, Germany
      Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, Ningbo 315201, Zhejiang, China
      More by Gang Wang
      Orcidhttps://orcid.org/0000-0002-9297-136X
    • Faxing Wang
      Faxing Wang
      Center for Advancing Electronics Dresden (cfaed) and Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Mommsenstr. 4, 01062 Dresden, Germany
      More by Faxing Wang
    • Zhiyong Wang
      Zhiyong Wang
      Center for Advancing Electronics Dresden (cfaed) and Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Mommsenstr. 4, 01062 Dresden, Germany
      Max Planck Institute of Microstructure Physics, D-06120 Halle (Saale), Germany
      More by Zhiyong Wang
    • Guangbo Chen
      Guangbo Chen
      Center for Advancing Electronics Dresden (cfaed) and Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Mommsenstr. 4, 01062 Dresden, Germany
      More by Guangbo Chen
    • Sheng Yang
      Sheng Yang
      Center for Advancing Electronics Dresden (cfaed) and Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Mommsenstr. 4, 01062 Dresden, Germany
      Frontiers Science Center for Transformative Molecules, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, 200240 Shanghai, China
      More by Sheng Yang
    • Youwen Liu
      Youwen Liu
      State Key Laboratory of Materials Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, 430074 Wuhan, China
      More by Youwen Liu
      Orcidhttps://orcid.org/0000-0001-9929-4616
    • Renhao Dong
      Renhao Dong
      Center for Advancing Electronics Dresden (cfaed) and Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Mommsenstr. 4, 01062 Dresden, Germany
      Key Laboratory of Colloid and Interface Chemistry of the Ministry of Education, School of Chemistry and Chemical Engineering, Shandong University, 250100 Jinan, China
      More by Renhao Dong
      Orcidhttps://orcid.org/0000-0002-4125-9284
    • Minghao Yu*
      Minghao Yu
      Center for Advancing Electronics Dresden (cfaed) and Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Mommsenstr. 4, 01062 Dresden, Germany
      *Email: [email protected]
      More by Minghao Yu
      Orcidhttps://orcid.org/0000-0002-0211-0778
    • Xing Lu
      Xing Lu
      State Key Laboratory of Materials Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, 430074 Wuhan, China
      More by Xing Lu
      Orcidhttps://orcid.org/0000-0003-2741-8733
    • Xinliang Feng*
      Xinliang Feng
      Center for Advancing Electronics Dresden (cfaed) and Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Mommsenstr. 4, 01062 Dresden, Germany
      Max Planck Institute of Microstructure Physics, D-06120 Halle (Saale), Germany
      *Email: [email protected]
      More by Xinliang Feng
      Orcidhttps://orcid.org/0000-0003-3885-2703
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    Cite this: J. Am. Chem. Soc. 2023, 145, 11, 6247–6256
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    https://doi.org/10.1021/jacs.2c12684
    Published March 9, 2023
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    Although two-dimensional conjugated metal–organic frameworks (2D c-MOFs) provide an ideal platform for precise tailoring of capacitive electrode materials, high-capacitance 2D c-MOFs for non-aqueous supercapacitors remain to be further explored. Herein, we report a novel phthalocyanine-based nickel-bis(dithiolene) (NiS4)-linked 2D c-MOF (denoted as Ni2[CuPcS8]) with outstanding pseudocapacitive properties in 1 M TEABF4/acetonitrile. Each NiS4 linkage is disclosed to reversibly accommodate two electrons, conferring the Ni2[CuPcS8] electrode a two-step Faradic reaction with a record-high specific capacitance among the reported 2D c-MOFs in non-aqueous electrolytes (312 F g–1) and remarkable cycling stability (93.5% after 10,000 cycles). Multiple analyses unveil that the unique electron-storage capability of Ni2[CuPcS8] originates from its localized lowest unoccupied molecular orbital (LUMO) over the nickel-bis(dithiolene) linkage, which allows the efficient delocalization of the injected electrons throughout the conjugated linkage units without inducing apparent bonding stress. The Ni2[CuPcS8] anode is used to demonstrate an asymmetric supercapacitor device that delivers a high operating voltage of 2.3 V, a maximum energy density of 57.4 Wh kg–1, and ultralong stability over 5000 cycles.

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    • Experimental methods, PXRD patterns, SEM images, XPS spectra, FT-IR spectra, XANES spectra, EXAFS spectra, HR-TEM images, electrochemical performance of Ni2[CuPcS8], Ni2[CuPc(NH)8], and Ni2[CuPcO8] electrodes, and performance comparison (PDF)

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    Cite this: J. Am. Chem. Soc. 2023, 145, 11, 6247–6256
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.2c12684
    Published March 9, 2023
    Copyright © 2023 American Chemical Society
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