期刊
NATURE COMMUNICATIONS
卷 12, 期 1, 页码 -出版社
NATURE PORTFOLIO
DOI: 10.1038/s41467-021-27127-5
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资金
- National Natural Science Foundation of China [21675084, 22073087]
- Natural Science Foundation of Jiangsu Province [BZ2021010]
- CAS Project for Young Scientists in Basic Research [YSBR-004]
- MOST [2018YFA0208603, 2016YFA0200602]
- Super Computer Centre of USTCSCC
- Super Computer Centre of SCCAS
This study demonstrates the efficient ECL emitter using a D-A COF with adjustable intrareticular charge transfer, leading to a significant enhancement in ECL intensity. The dual-peaked ECL patterns of COFs are achieved through an IRCT mediated competitive oxidation mechanism, providing new insights for designing next-generation ECL devices.
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. Controlling the charge transfer between radical anions and cations is a promising way to tune the emission mechanism in electrochemiluminescence (ECL) systems. Here, the authors report a donor-acceptor based covalent organic framework, using triphenylamine and triazine building units, and demonstrate efficient ECL based on an adjustable intrareticular charge transfer.
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