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

Rengan Luo, Haifeng Lv, Qiaobo Liao, Ningning Wang, Jiarui Yang, Yang Li, Kai Xi (), Xiaojun Wu (), Huangxian Ju and Jianping Lei ()
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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

Nature Communications, 2021, vol. 12, issue 1, 1-9

Abstract: 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.

Date: 2021
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DOI: 10.1038/s41467-021-27127-5

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