College of Chemistry, Beijing Normal University, Beijing 100875, PR China.
Beijing National Laboratory for Molecular Sciences, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, PR China.
Anal Chim Acta. 2018 Mar 20;1003:49-55. doi: 10.1016/j.aca.2017.11.068. Epub 2017 Dec 12.
In this work, we developed a sensitive and highly selective fluorescent approach for the detection of ascorbic acid (AA) by taking advantage of the oxidative etching effect of iodine (I) on the lysozyme-stabilized silver nanoclusters (dLys-AgNCs) with fluorescence quenching. I could be produced from the redox reaction between iodate (IO) and AA, and thus the fluorescence intensity of dLys-AgNCs was turned off significantly in the coexistence of IO and AA. The fluorescence quenching of dLys-AgNCs had a good linear relationship with AA concentration, which allowed the detection of AA in the range from 0.05 to 45.0 μmol L with a detection limit of 20 nmol L. The quenching mechanism was elucidated by Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), zeta potential, and dynamic light scattering (DLS) measurements, confirming that the fluorescence quenching of the dLys-AgNCs was attributed to the oxidative etching of the in situ generated I, inducing aggregation of the dLys-AgNCs probe by forming Ag@AgI nanocomposite. The dLys-AgNCs probe exhibited excellent selectivity for AA sensing over several common reducing agents tested. Moreover, this approach was extended to the detection of AA in orange juice and urine with recovery rates in the range of 96.0% (RSD: 4.11) to 100.9% (RSD: 3.28) and 94.5% (RSD: 6.40) to 99.2% (RSD: 5.36), respectively.
在这项工作中,我们利用碘(I)对溶菌酶稳定的银纳米簇(dLys-AgNCs)的氧化蚀刻效应,开发了一种灵敏且高度选择性的荧光方法来检测抗坏血酸(AA)。I 可以通过碘酸盐(IO)和 AA 之间的氧化还原反应产生,因此在 IO 和 AA 共存的情况下,dLys-AgNCs 的荧光强度显著猝灭。dLys-AgNCs 的荧光猝灭与 AA 浓度呈良好的线性关系,允许在 0.05 至 45.0 μmol L 的范围内检测 AA,检测限为 20 nmol L。傅里叶变换红外光谱(FTIR)、X 射线光电子能谱(XPS)、透射电子显微镜(TEM)、Zeta 电位和动态光散射(DLS)测量阐明了猝灭机制,证实了 dLys-AgNCs 的荧光猝灭归因于原位生成的 I 的氧化蚀刻,通过形成 Ag@AgI 纳米复合材料诱导 dLys-AgNCs 探针聚集。与测试的几种常见还原剂相比,dLys-AgNCs 探针对 AA 传感具有优异的选择性。此外,该方法还扩展到橙汁和尿液中 AA 的检测,回收率在 96.0%(RSD:4.11)至 100.9%(RSD:3.28)和 94.5%(RSD:6.40)至 99.2%(RSD:5.36)范围内。