Wang Kai, Ru Zongling, Shi Jiwei, Zhu Yuezhao, Yang Liguo, Wei Mengxue, Xiao Mengli, Liu Nana, Wang Fang
School of Chemical and Environmental Engineering, Anyang Institute of Technology Anyang 455000 China
School of Materials Science and Engineering, Anyang Institute of Technology Anyang 455000 China.
RSC Adv. 2022 Sep 26;12(42):27170-27178. doi: 10.1039/d2ra04477c. eCollection 2022 Sep 22.
Great advances have been made in the development of carbon dot (CD)-based fluorescent materials for the detection of hypochlorite in the past few years. However, developing new CDs with high quantum yield (QY) for the rapid detection of hypochlorite and gaining a deeper insight into the detection mechanism still need to be further investigated. Herein, N-doped carbon dots (NCDs) with high QYs, which can reach as high as 67%, were efficiently prepared employing citric acid and -phenylenediamine as raw materials. Significantly, the NCDs could act as fluorescent probes for the rapid detection of hypochlorite and the limit of detection is calculated to be as low as 12.6 nM on the basis of fluorescent "on-off" effects upon the addition of hypochlorite. Furthermore, UV-vis absorption spectra, Density Functional Theory (DFT) calculations and kinetic analysis of fluorescence (FL) decay were used to investigate the detection mechanism. The results indicate that the electron transfer (ET) process from NCDs to imine-functionalized NCDs (imine-NCDs) and the higher energy gap of imine-NCDs will facilitate the excited-energy of NCDs to be dissipated in the form of a non-radiative decay procedure, resulting in a static quenching mechanism. Therefore, these observations are useful in deepening the understanding of the hypochlorite induced FL quenching mechanism and thereby developing oxidative stress-related detection materials.
在过去几年中,基于碳点(CD)的荧光材料用于次氯酸盐检测方面取得了巨大进展。然而,开发具有高量子产率(QY)的新型碳点以快速检测次氯酸盐并更深入地了解检测机制仍有待进一步研究。在此,以柠檬酸和对苯二胺为原料,高效制备了量子产率高达67%的N掺杂碳点(NCDs)。值得注意的是,NCDs可作为荧光探针用于快速检测次氯酸盐,基于加入次氯酸盐后的荧光“开-关”效应,计算出检测限低至12.6 nM。此外,利用紫外可见吸收光谱、密度泛函理论(DFT)计算和荧光(FL)衰减动力学分析来研究检测机制。结果表明,从NCDs到亚胺功能化NCDs(imine-NCDs)的电子转移(ET)过程以及imine-NCDs的较高能隙将促进NCDs的激发能以非辐射衰减过程的形式耗散,从而导致静态猝灭机制。因此,这些观察结果有助于加深对次氯酸盐诱导的荧光猝灭机制的理解,进而开发与氧化应激相关的检测材料。