上转换荧光传感检测赭曲霉毒素A的研究（英文）
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摘要
本文基于分子印迹技术的高选择性和上转换纳米材料的荧光特性,以赭曲霉毒素A(OTA)的结构类似物HNA-Phe为模板,开发了一种能高选择、高灵敏地识别痕量OTA的分子印迹聚合物(UCNPs@SiO_2@MIP)。在最优条件下,当OTA浓度为0.05～1.0 mg/L时,荧光印迹聚合物的荧光猝灭程度与OTA的浓度呈现良好的线性关系。建立了OTA的荧光传感检测方法,该方法的最低检出限为0.031mg/L。当OTA的加标浓度为50、100和200μg/kg时,大米、玉米和饲料中OTA的回收范围分别为80.2%～91.6%(RSD<4.6%)、89.2%～90.4%(RSD<5.5%)和88.0%～91.6%(RSD<5.4%)。
A novel molecularly imprinted polymer(MIP) based on upconversion nanoparticles(UCNPs) was successfully synthesized for determination of Ochratoxin A(OTA). The MIP was developed on the silica-coated UCNPs using N-(1-hydroxy-2-naphthoyl amido)-(L)-phenylalanine(HNA-Phe) as the alternative template. The final composite combined the advantages of the high selectivity of MIP with the high fluorescence intensity of UCNPs which was selective and sensitive to OTA. Under the optimal condition, the fluorescence intensity of UCNPs@SiO_2@MIP decreases linearly when the concentration of OTA increases from 0.05 to 1.0 mg/L. The detection limit of OTA with the method was 0.031 mg/L. At three spiked concentration levels(50, 100 and 200 μg/kg), the recovery ranges of OTA in corn, rice and feed are 88.0%–91.6%, 80.2%–91.6% and 89.2%–90.4%, respectively.
A novel molecularly imprinted polymer(MIP) based on upconversion nanoparticles(UCNPs) was successfully synthesized for determination of Ochratoxin A(OTA). The MIP was developed on the silica-coated UCNPs using N-(1-hydroxy-2-naphthoyl amido)-(L)-phenylalanine(HNA-Phe) as the alternative template. The final composite combined the advantages of the high selectivity of MIP with the high fluorescence intensity of UCNPs which was selective and sensitive to OTA. Under the optimal condition, the fluorescence intensity of UCNPs@SiO_2@MIP decreases linearly when the concentration of OTA increases from 0.05 to 1.0 mg/L. The detection limit of OTA with the method was 0.031 mg/L. At three spiked concentration levels(50, 100 and 200 μg/kg), the recovery ranges of OTA in corn, rice and feed are 88.0%–91.6%, 80.2%–91.6% and 89.2%–90.4%, respectively.
引文
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[26]ZHANG Fang,WAN Ying,YU Ting,ZHANG Fu-qiang,SHI Yi-feng,XIE Song-hai,LI Yi-gang,XU Lei,TU Bo,ZHAO Dong-yuan.Uniform nanostructured arrays of sodium rare-earth fluorides for highly efficient multicolor upconversion luminescence[J].Angewandte Chemie International Edition,2007,119(42):7976-7979.DOI:10.1002/anie.200702519.
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[28]LIU Hui-lin,FANG Guo-zhen,ZHU Hui-dan,LI Chang-mo,LIU Cui-cui,WANG Shuo.A novel ionic liquid stabilized molecularly imprinted optosensing material based on quantum dots and graphene oxide for specific recognition of vitamin E[J].Biosensors&Bioelectronics,2013,47(10):127-132.DOI:https://doi.org/10.1016/j.bios.2013.03.006.
[2]MANTLE P G.Rat kidney cancers determined by dietary Ochratoxin A in the first year of life[J].Journal of Kidney Cancer&VHL,2016,3(3):1-10.DOI:10.15586/jkcvhl.2016.58.
[3]XIONG Ke,WANG Xiao-ling,ZHI Hui-wei,SUN Bao-guo,LI Xiu-ting.Identification and safety evaluation of a product from biodegradation of ochratoxin a by an aspergillus strain[J].Journal of the Science of Food&Agriculture,2016,97(2):434-443.DOI:10.1002/jsfa.7742.
[4]WOO C S J,EL-NEZAMI H.Maternal-fetal cancer risk assessment of Ochratoxin A during pregnancy[J].Toxins,2016,8(4):1-16.DOI:10.3390/toxins8040087.
[5]PALUMBO J D,O'KEEFFE T L,HO Y S,SANTILLAN C J.Occurrence of Ochratoxin A contamination and detection of Ochratoxigenic aspergillus species in retail samples of dried fruits and nuts[J].Journal of Food Protection,2015,78(4):836-842.DOI:10.4315/0362-028X.JFP-14-471.
[6]OKUMA T A,HUYNH T P,HELLBERG R S.Use of enzyme-linked immunosorbent assay to screen for aflatoxins,Ochratoxin A,and deoxynivalenol in dry pet foods[J].Mycotoxin Research,2018,34(1):69-75.DOI:https://doi.org/10.1007/s12550-017-0300-3.
[7]LAU B P Y,SCOTT P M,LEWIS D A,KANHERE S R.Quantitative determination of Ochratoxin A by liquid chromatography/electrospray tandem mass spectrometry[J].Journal of Mass Spectrometry,2000,35(1):23-32.DOI:10.1002/(SICI)1096-9888(200001)35:1<23::AID-JMS903>3.0.CO;2-B.
[8]WANG Pei-long,SUN Xiao-hua,SU Xiao-ou,WANG Tie.Advancements of molecularly imprinted polymers in the food safety field[J].Analyst,2016,141(12):3540-3553.DOI:10.1039/c5an01993a.
[9]NEZHADALI A,FEIZY J,BEHESHTI H R.A molecularly imprinted polymer for the selective extraction and determination of fenvalerate from food samples using high-performance liquid chromatography[J].Food Analytical Methods,2015,8(5):1225-1237.DOI:10.1007/s12161-014-0004-7.
[10]YOLA M L,GUPTA V K,ATAR N.New molecular imprinted voltammetric sensor for determination of Ochratoxin A[J].Materials Science&Engineering C,2016,61:368-375.DOI:10.1016/j.msec.2015.12.057.
[11]CAO Ji-liang,KONG Wei-jun,ZHOU Shu-jun,YIN Li-hui,WAN Li,YANG Mei-hua.Molecularly imprinted polymer-based solid phase clean-up for analysis of Ochratoxin A in beer,red wine,and grape juice[J].Journal of Separation Science,2013,36(7):1291-1297.DOI:10.1002/jssc.201201055.
[12]HONG Chao-ma,LI Hai-pu,YANG Zhao-guang,XUQian-jin,MA Li.Preparation and property of environmental hormone 17β-estradiol molecularly imprinted polymers[J].Journal of Central South University:Science and Techaology,2014,45(5):1403-1410.(in Chinese)
[13]ZHAN Jie,FANG Guo-zhen,YAN Zhen,PAN Ming-fei,LIU Cui-cui.Preparation of a semicovalent,molecularly surface imprinted polymer for the rapid determination of trace acid orange II in food and environmental samples[J].Analytical&Bioanalytical Chemistry,2013,405(19):6353-6363.DOI:10.1007/s00216-013-7036-5.
[14]YANG Yan,MENG Xiang-jun,XIAO Zheng-gang.Synthesis of a surface molecular imprinting polymer based on silica and its application in the identification of nitrocellulose[J].Rsc Advances,2018,8(18):9802-9811.DOI:10.1039/c7ra13264f.
[15]FANG Guo-zhen,FAN Chao,LIU Hui-lin,PAN Ming-fei,ZHU Hui-dan,WANG Shuo.A novel molecularly imprinted polymer on Cd Se/Zn S quantum dots for highly selective optosensing of mycotoxin zearalenone in cereal samples[J].Rsc Advances,2013,4(6):2764-2771.DOI:10.1039/c2jm33522k.
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[17]GUO Ting,DENG Qi-liang,FANG Guo-zhen,LIU Cui-cui,HUANG Xuan,WANG Shuo.Molecularly imprinted upconversion nanoparticles for highly selective and sensitive sensing of Cytochrome c[J].Biosensors&Bioelectronics,2015,74:498-503.DOI:10.1016/j.bios.2015.06.058.
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[19]LIU Yu-jia,LU Yi-qing,YANG Xu-san,ZHENG Xian-lin,WEN Shi-hui,WANG Fan,VIDAL X,ZHAO Jiang-bo,LIUDe-ming,ZHOU Zhi-guang.Amplified stimulated emission in upconversion nanoparticles for super-resolution nanoscopy[J].Nature,2017,543(7644):229-233.DOI:10.1038/nature21366.
[20]LV Jia-jia,ZHAO Sen,WU Shi-jia,WANG Zhou-ping.Upconversion nanoparticles grafted molybdenum disulfide nanosheets platform for microcystin-LR sensing[J].Biosensors&Bioelectronics,2017,90(15):203-209.DOI:10.1016/j.bios.2016.09.110.
[21]CHEN Guo-jun,RENATA J S,ESQUIBEL C R,LOU I,ZHENG Qi-feng,DAMMALAPATI A,HARRISON A,ELICEIRI K W,TANG Wei-ping,CHEN H.Neuroendocrine Tumor-targeted upconversion nanoparticle-based micelles for simultaneous nir-controlled combination chemotherapy and photodynamic therapy,and fluorescence imaging[J].Advanced Functional Materials,2017,27(8):1-13.DOI:10.1002/adfm.201604671.
[22]WU S,BUTT H J.Near-infrared-sensitive materials based on upconverting nanoparticles[J].Advanced Materials,2016,28(6):1208-1226.DOI:10.1002/adma.201502843.
[23]LIU Xiao-lin,ZHANG Ning,LI Dan,LI Zhi-cheng,YOUWei-xiong,ZHANG Qian,XIA Li-bin,YANG Bin.Fuel combustion synthesis and upconversion properties of Yb3+and Er3+dual-doped ZrO2 nanocrystals[J].Journal of Central South University,2017,24(10):2209-2214.DOI:10.1007/s11771-017-3629-z.
[24]QIAN Kun,FANG Guo-zhen,WANG Shuo.Highly sensitive and selective novel core-shell molecularly imprinted polymer based on NaYF4:Yb3+,Er3+upconversion fluorescent nanorods[J].Rsc Advances,2013,3(12):3825-3828.DOI:10.1039/c3ra23003a.
[25]BAGGIANI C,BIAGIOLI F,ANFOSSI L,GIOVANNOLIC,PASSINI C,GIRAUDI G.Effect of the mimic structure on the molecular recognition properties of molecularly imprinted polymers for Ochratoxin A prepared by a fragmental approach[J].Reactive&Functional Polymers,2013,73(6):833-837.DOI:10.1016/j.reactfunctpolym.2013.03.018.
[26]ZHANG Fang,WAN Ying,YU Ting,ZHANG Fu-qiang,SHI Yi-feng,XIE Song-hai,LI Yi-gang,XU Lei,TU Bo,ZHAO Dong-yuan.Uniform nanostructured arrays of sodium rare-earth fluorides for highly efficient multicolor upconversion luminescence[J].Angewandte Chemie International Edition,2007,119(42):7976-7979.DOI:10.1002/anie.200702519.
[27]MADER H S,LINK M,ACHATZ D E,UHLMANN K,LIXiao-hua,WOLFBEIS O S.Surface-modified upconverting microparticles and nanoparticles for use in click chemistries[J].Chemistry-A European Journal,2010,16(18):5416-5424.DOI:10.1002/chem.201000117.
[28]LIU Hui-lin,FANG Guo-zhen,ZHU Hui-dan,LI Chang-mo,LIU Cui-cui,WANG Shuo.A novel ionic liquid stabilized molecularly imprinted optosensing material based on quantum dots and graphene oxide for specific recognition of vitamin E[J].Biosensors&Bioelectronics,2013,47(10):127-132.DOI:https://doi.org/10.1016/j.bios.2013.03.006.