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As an attractive electrochemiluminescence (ECL) emitter, graphitic carbon nitride (CN) still suffers from weak and unstable ECL signals for its poor conductivity and the occurrence of electrode passivation. In this study, a simple nitrogen vacancy (NV) engineering strategy has been developed for the improvement of ECL performances (intensity and stability) for the first time. In comparison to pristine CN (RSD = 51.98% for 10 continuous scan), ca. 60 times amplification in ECL intensity and 70 times enhancement in ECL efficiency for CN modified with NVs (CN-NVs) were obtained. In addition, more stable ECL emissions (RSD = 0.53%) were achieved for CN-NV-550 by thermal treatment of pristine CN in a N2 atmosphere for another 2 h at 550 °C. The mechanism study for the vital role of NVs on the ECL of CN-NVs revealed that NVs can not only facilitate electron transfer to amplify the ECL intensity but also serve as the electron trap to inhibit electrode passivation. More interestingly, a series of CN-NVs exhibited a tunable ECL wavelength range from 470 to 516 nm with different NV contents. Moreover, their ECL spectra showed an obvious red-shift of the wavelength with their corresponding fluorescence spectra. These findings confirmed that the ECL emissions of CN-NVs were susceptible to the relevant surface states of NVs. Our work may open up a promising pathway for improving ECL performances of CN and create new possibilities for multitarget simultaneous detection based on ECL and construction of color tunable light-emitting devices.
Zou et al. (Mon,) studied this question.