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Intrareticular charge transfer regulated electrochemiluminescence of donor–acceptor covalent organic frameworks

Author

Listed:
  • Rengan Luo

    (State Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry and Chemical Engineering, Nanjing University)

  • Haifeng Lv

    (Hefei National Laboratory for Physical Sciences at the Microscale, Synergetic Innovation of Quantum Information and Quantum Technology, CAS Center for Excellence in Nanoscience, and School of Chemistry and Materials Sciences, University of Science and Technology of China)

  • Qiaobo Liao

    (School of Chemistry and Chemical Engineering, Nanjing University)

  • Ningning Wang

    (State Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry and Chemical Engineering, Nanjing University)

  • Jiarui Yang

    (State Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry and Chemical Engineering, Nanjing University)

  • Yang Li

    (State Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry and Chemical Engineering, Nanjing University)

  • Kai Xi

    (School of Chemistry and Chemical Engineering, Nanjing University)

  • Xiaojun Wu

    (Hefei National Laboratory for Physical Sciences at the Microscale, Synergetic Innovation of Quantum Information and Quantum Technology, CAS Center for Excellence in Nanoscience, and School of Chemistry and Materials Sciences, University of Science and Technology of China)

  • Huangxian Ju

    (State Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry and Chemical Engineering, Nanjing University)

  • Jianping Lei

    (State Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry and Chemical Engineering, Nanjing University)

Abstract

The control of charge transfer between radical anions and cations is a promising way for decoding the emission mechanism in electrochemiluminescence (ECL) systems. Herein, a type of donor-acceptor (D-A) covalent organic framework (COF) with triphenylamine and triazine units is designed as a highly efficient ECL emitter with tunable intrareticular charge transfer (IRCT). The D-A COF demonstrates 123 folds enhancement in ECL intensity compared with its benzene-based COF with small D-A contrast. Further, the COF’s crystallinity- and protonation-modulated ECL behaviors confirm ECL dependence on intrareticular charge transfer between donor and acceptor units, which is rationalized by density functional theory. Significantly, dual-peaked ECL patterns of COFs are achieved through an IRCT mediated competitive oxidation mechanism: the coreactant-mediated oxidation at lower potential and the direct oxidation at higher potential. This work provides a new fundamental and approach to improve the ECL efficiency for designing next-generation ECL devices.

Suggested Citation

  • Rengan Luo & Haifeng Lv & Qiaobo Liao & Ningning Wang & Jiarui Yang & Yang Li & Kai Xi & Xiaojun Wu & Huangxian Ju & Jianping Lei, 2021. "Intrareticular charge transfer regulated electrochemiluminescence of donor–acceptor covalent organic frameworks," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-27127-5
    DOI: 10.1038/s41467-021-27127-5
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    References listed on IDEAS

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