金磁纳米颗粒的制备及其在表面增强拉曼光谱快速检测黄曲霉毒素B1中的应用
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摘要
本文采用纳米Fe_3O_4颗粒作为磁性核心,先用四乙氧基硅烷、再用3-巯丙基三乙氧基硅烷和3-氨丙基三乙氧基硅烷修饰Fe_3O_4颗粒,形成表面带-NH_2和-SH的Fe_3O_4/SiO_2纳米颗粒,进一步通过-NH_2的静电吸附和Au-S键的作用将金纳米颗粒组装在Fe_3O_4/SiO_2表面,形成具有核壳结构的Fe_3O_4/SiO_2/Au金磁纳米颗粒,并用透射电子显微镜镜(TEM)、能量色散X射线光谱仪(EDX)、紫外可见分光光度计(UV-vis)等技术对金磁纳米颗粒进行了形貌观测及性质表征。利用Fe_3O_4/SiO_2/Au金磁纳米颗粒作为拉曼活性基底,用表面增强拉曼光谱仪对黄曲霉毒素B1(AFB1)进行直接快速检测,发现无外磁体浓缩的情况下AFB1的检测限大于10.0μg/m L,在外磁体浓缩金磁纳米颗粒的情况下检测限降低100倍(≤0.1μg/m L),检测线性范围0.1μg/m L~10.0μg/m L,检测的样品回收率为84.35%~91.98%,相对标准偏差在4.88%~9.90%之间。
To introduce-NH_2 and-SH to the surface of Fe_3O_4/SiO_2 nanoparticles, Fe_3O_4 nanoparticles were first modified with tetraethoxylsilane to form Fe_3O_4/SiO_2 nanoparticles, followed by the addition of 3-thiolpropyltriethxoysilane and 3-aminopropyltriethxoysilane. Au nanoparticles were then assembled on the surface of Fe_3O_4/SiO_2 via the electrostatic adsorption of-NH_2 and the effect of the Au-S bond to produce core-shell Fe_3O_4/SiO_2/Au gold magnetic nanoparticles. These magnetic nanoparticles were characterized by a variety of techniques such as transmission electron microscopy(TEM), energy dispersive X-ray spectrometer(EDX) and ultraviolet spectrophotometer(UV-vis). Using Fe_3O_4/SiO_2/Au gold magnetic nanoparticles as a Raman active substrate, aflatoxin B1(AFB1) was directly and rapidly detected by surface-enhanced Raman spectrometry. In the absence of external magnetic concentration of gold magnetic nanoparticles, the detection limit of AFB1 was higher than 10.0 μg/m L, while in the presence of external magnetic concentration, the detection limit was decreased 100-fold(≤0.1 μg/m L) with a linear detection range of 0.1~10.0 μg/m L. The recovery rate of samples was 84.35~91.98% and the relative standard deviation was 4.88~9.90%.
To introduce-NH_2 and-SH to the surface of Fe_3O_4/SiO_2 nanoparticles, Fe_3O_4 nanoparticles were first modified with tetraethoxylsilane to form Fe_3O_4/SiO_2 nanoparticles, followed by the addition of 3-thiolpropyltriethxoysilane and 3-aminopropyltriethxoysilane. Au nanoparticles were then assembled on the surface of Fe_3O_4/SiO_2 via the electrostatic adsorption of-NH_2 and the effect of the Au-S bond to produce core-shell Fe_3O_4/SiO_2/Au gold magnetic nanoparticles. These magnetic nanoparticles were characterized by a variety of techniques such as transmission electron microscopy(TEM), energy dispersive X-ray spectrometer(EDX) and ultraviolet spectrophotometer(UV-vis). Using Fe_3O_4/SiO_2/Au gold magnetic nanoparticles as a Raman active substrate, aflatoxin B1(AFB1) was directly and rapidly detected by surface-enhanced Raman spectrometry. In the absence of external magnetic concentration of gold magnetic nanoparticles, the detection limit of AFB1 was higher than 10.0 μg/m L, while in the presence of external magnetic concentration, the detection limit was decreased 100-fold(≤0.1 μg/m L) with a linear detection range of 0.1~10.0 μg/m L. The recovery rate of samples was 84.35~91.98% and the relative standard deviation was 4.88~9.90%.
引文
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[2]Vdovenko M M,Lu C C,Yu F Y,et al.Development of ultrasensitive direct chemiluminescent enzyme immunoassay for determination of aflatoxin B1 in food products[J].Talanta,2013,107(5):25-29
[3]International agency for research on cancer(IARC).Aflatoxins,some naturally occurring substances:food items and constituents,heterocyclic aromatic amines and mycotoxins[M].IARC,Lyon France,1993:245-395
[4]Durnez L,Bortel W V,Denis L,et al.False positive circumsporozoite protein ELISA:a challenge for the estimation of the entomological inoculation rate of malaria and for vector incrimination[J].Malaria Journal,2011,10(29):1-9
[5]Jeanmaire D L,Duyne R P V,Jeanmaire D L,et al.Surface Raman spectroelectrochemistry:Part I.Heterocyclic,aromatic,and aliphatic amines adsorbed on the anodized silver electrode[J].Journal of Electroanalytical Chemistry&Interfacial Electrochemistry,1977,84(1):1-20
[6]Albrecht M G,Creighton J A.Anomalously intense Raman spectra of pyridine at a silver electrode[J].Journal of the American Chemical Society,2002,99(15):5215-5217
[7]Lu G,Li H,Liusman C,et al.Surface enhanced Raman scattering of Ag or Au nanoparticle-decorated reduced graphene oxide for detection of aromatic molecules[J].Chemical Science,2011,2(9):1817-1821
[8]Fleischmann M,Hendra P J,Mcquillan A J.Raman spectra of pyridine adsorbed at a silver electrode[J].Chemical Physics Letters,1974,26(2):163-166
[9]Mirzabe G H,Keshtkar A R.Application of response surface methodology for thorium adsorption on PVA/Fe3O4/Si O2/APTES nanohybrid adsorbent[J].Journal of Industrial and Engineering Chemistry,2015,26:277-285
[10]Chao H,Chengmin S,Jifa T,et al.Core-shell Fe3O4@Si O2nanoparticles synthesized with well-dispersed hydrophilic Fe3O4 seeds[J].Nanoscale,2011,3(2):701-705
[11]Wu H Y,Huang W L,Huang M H.Direct high-yield synthesis of high aspect ratio gold nanorods[J].Crystal Growth&Design,2007,7(4):831-835
[12]高思敏,王红艳,林月霞,等.黄曲霉素B1在银团簇表面吸附的表面增强拉曼光谱[J].物理化学学报,2012,28(9):2044-2050GAO Si-min,WANG Hong-yan,LIN Yue-xia,et al.Surface-enhanced Raman spectra of aflatoxin B1 adsorbed on silver clusters[J].Acta Physico-Chimica Sinica,2012,28(9):2044-2050
[13]Hakonen A,Andersson P O,Schmidt M S,et al.Explosive and chemical threat detection by surface-enhanced raman scattering:A review[J].Analytica Chimica Acta,2015,893:1-13
[14]潘晓会,张芹,郭伟,等.利用AAO模板制备SERS基底检测Sudan I[J].光谱学与光谱分析,2015,35(6):1556-1561PAN Xiao-hui,ZHANG Qin,GUO Wei,et al.The SERS detection of Sudan I by using AAO as a template to prepare SERS substrate[J].Spectroscopy and Spectral Analysis,2015,35(6):1556-1561