Trace Detection of Rhodamine B in Infant Candy by g-C3N4/Ag Nanocomposite as Surface-Enhanced Raman Scattering Substrate

doi:10.6023/A19050191

Abstract

In recent years, food safety problems caused by illegal additions in infant foods have received widespread attention. Surface-enhanced Raman scattering (SERS) technique is used to rapidly and non-destructively detect the banned RhB that is usually added in food. In this study, we have prepared g-C₃N₄/Ag composites via a simple method successfully, their morphology and structure were characterized by transmission electron microscope (TEM), ultraviolet-visible (UV-Vis), X-ray diffraction (XRD), fluorescence spectrophotometer and confocal micro-Raman spectrometer (Raman). The g-C₃N₄ nanosheet possesses good adsorption performance due to its highly delocalized π-conjugated system, which acts as a carrier for Ag nanoparticles. Therefore, Ag nanoparticles are more uniformly and stably distributed on the surface of g-C₃N₄ nanosheets to form g-C₃N₄/Ag nanocomposite, which can be used for rapid adsorption and trace detection of RhB. In the experiment, the pH of the test and the absorbed time between the substrate and RhB were optimized. The influence of pH on the SPR of the substrate and the SERS intensity of the probe molecule were investigated in detail. As g-C₃N₄/Ag nanocomposite shows a significant higher absorption in the visible region around 500 nm than Ag nanoparticles, g-C₃N₄/Ag nanocomposite is more favorable for SPR absorption. A wide SPR absorption range is achieved due to the synergy between g-C₃N₄ and Ag nanoparticles, providing an improved SERS enhancement performance. Under the optimal experimental conditions by using RhB as probe molecule, an enhancement factor of 7.6×10 ⁵ is achieved. Due to the electrostatic interaction and π-π interaction between the substrate and the probe molecules, the substrate can enrich in a large amount of cationic dyes, offering a detection of RhB. The g-C₃N₄/Ag SERS substrate can be used to detect RhB with a linear relationship from 1.0×10 ^–9 to 1.0×10 ^–6 mol/L and a detection limit as low as 0.39 nmol/L. In addition, the g-C₃N₄/Ag nanocomposite SERS substrate can also detect trace amounts of RhB molecules in the commercially available rainbow lollipops with a high sensitivity, and the recovery were 93.6%~95.04%. In summary, the g-C₃N₄/Ag nanocomposite is not only a SERS substrate with high sensitivity, uniformity and stability, but also can be used as a rapid trace detection method of Rhodamine B in real food and environment.

Key words: surface enhanced Raman spectroscopy (SERS), g-C₃N₄/Ag nanocomposites, Rhodamine B, candy, trace detection

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Ma, Chao, Wu, Jiawei, Zhu, Lin, Han, Xiaoxia, Ruan, Weidong, Song, Wei, Wang, Xu, Zhao, Bing. Trace Detection of Rhodamine B in Infant Candy by g-C₃N₄/Ag Nanocomposite as Surface-Enhanced Raman Scattering Substrate[J]. Acta Chimica Sinica, 2019, 77(10): 1024-1030.

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Fig. & Tab. 8

Figure 1. Characterization of g-C3N4/Ag nanocomposites. (a), (b), (c) TEM images of g-C3N4 nanosheets, Ag nanoparticles and g-C3N4/Ag nanocomposites; (d) XRD patterns of g-C3N4 nanosheets and g-C3N4/Ag nanocomposites; (e) Photoluminescence spectra of silver nanoparticles, g-C3N4 nanosheets and g-C3N4/Ag nanocomposites; (f) Raman spectra of g-C3N4 nanosheets and g-C3N4/Ag nanocomposites

Figure 2. (a) UV-visible absorption spectra of silver nanoparticles, g-C3N4 nanosheets, g-C3N4/Ag nanocomposites and UV-visible absorption differential spectra of g-C3N4/Ag nanocomposites and silver nanoparticles; (b) SERS spectra of 5×10–7 mol/L RhB adsorbed on g-C3N4/Ag nanocomposites, Ag nanoparticles, and Raman spectra of 0.01 mol/L RhB solution

Figure 3. (a) A series of SERS spectra of RhB (5×10–7 mol/L) molecules from 25 different spots on the SERS active substrates and the relative standard deviation (RSD) of SERS characteristic peaks intensities of RhB (b)1645 cm–1, (c) 1355 cm–1, (d) 1276 cm–1; (e), (f) SERS spectra of RhB solution with adsorption concentration of 1×10–6 mol/L at different times

Figure 4. (a) SERS spectra of RhB (1.0×10–6 mol/L) in the different pH (1.87, 2.26, 3.41, 4.15, 5.66, 6.67) with g-C3N4/Ag nanocomposites substrate; (b) tendency of the SERS intensity at 1645 cm–1 with a different pH value; (c) UV-visible absorption spectra of g-C3N4/Ag nanocomposites at different pH; (d) SERS spectra of RhB, Sudan Red, Orange 2, Acid Red (1.0×10–6 mol/L) in pH 2.26 with g-C3N4/Ag nanocomposites substrate

Figure 5. (a) SERS spectra of RhB (1.0×10–6 mol/L) in the different time with g-C3N4/Ag nanocomposites substrate; (b) tendency of the SERS intensity at 1645 cm–1 with a different time

Figure 6. (a) Surface-enhanced resonance Raman spectra of RhB with g-C3N4/Ag nanocomposites substrate, pH=2.26, 25 min (concentrations of RhB: 1.0×10–6, 5.0×10–7, 1.0×10–7, 5.0×10–8, 1.0×10–8, 5.0× 10–9, 1.0×10–9 mol/L); (b) the relationship between the intensity and the concentration of RhB

样品	添加/(μg?g^–1)	发现/(μg?g^–1)	回收率/%	RSD/%
彩虹棒棒糖	0.5 1.0	0.47 0.954	93.6 95.4	5.24 4.57

Table 1. Analytical results for the real samples

Figure 7. Schematic diagram of the preparation process

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g-C₃N₄/Ag纳米复合材料表面增强拉曼基底对婴幼儿糖果中的罗丹明B的痕量检测

Trace Detection of Rhodamine B in Infant Candy by g-C₃N₄/Ag Nanocomposite as Surface-Enhanced Raman Scattering Substrate

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g-C3N4/Ag纳米复合材料表面增强拉曼基底对婴幼儿糖果中的罗丹明B的痕量检测