摘要
微囊藻毒素-LR(MC-LR)具有强烈的肝毒性、致癌性和发育毒性,亟需严格监测。为实现环境水体中微痕量MC-LR的快速特异灵敏的分析识别,以金属有机框架化合物(MOF)为介导,增强磁纳米粒子比表面积,高效负载纳米金和适配体-cDNA分子杂交荧光探针,研发新型的适配体功能化磁纳米荧光探针(Fe3O4@MIL-101-NH2@Au@aptamer),实现了对MC-LR的适配体特异识别-激光诱导荧光(LIF)超高灵敏分析。论文详细研究了适配体磁纳米探针荧光检测MC-LR的可行性、 MC-LR测定的优化条件及其方法性能。结果表明:MOF修饰的磁纳米颗粒Fe3O4@MIL-101-NH2的Brunauer-Emmett-Teller(BET)比表面积达到114.02 m^(2)·g^(-1),比单一Fe3O4提高了近5倍,适配体-cDNA杂交荧光探针在磁纳米颗粒表面的修饰率达98%以上,适配体磁纳米探针对水体中痕量MC-LR具有很强的荧光响应。在最优条件下(pH 7.5、 NaCl浓度500 mmol·L^(-1)、纳米金尺寸为20 nm,测定时间为30 min),适配体磁纳米探针与MC-LR结合释放出荧光互补链,体系荧光强度与MC-LR含量成正比,线性浓度范围为0.020~3.000μg·L^(-1),检出限(LOD)为0.006μg·L^(-1),灵敏度比文献报道的荧光分析法提高了1.6~22.3倍。所建立的适配体磁纳米探针-LIF法对MC-LR的识别特异性高,在100倍量的干扰物(微囊藻毒素MC-RR、 MC-YR、大田软海绵酸OA)共存情况下,适配体磁纳米探针在混合体系中的荧光响应与在MC-LR单样中的响应强度偏差小于3.3%,交叉反应性小;日内、日间和批间的测定标准偏差(RSD)为1.7%~8.8%,相对误差RE为-4.3%~4.1%,方法稳定性和重现性好。该方法应用于闽江、西湖水和内河水等样品分析,水中MC-LR得到了良好的识别检出,不同加标浓度的MC-LR(0.050, 0.100和1.000μg·L^(-1))测定回收率为(90.1%±6.4%)~(104.2%±7.0%)(n=3),与LC-MS确证方法的测定结果[加标回收率(91.3%±7.0%)~(104.4%±2.0%),n=3]一致。所建立的适配体磁纳米探针与L
MC-LR possessing strong hepatotoxicity,potential carcinogenicity,and biolog ical toxicity could have an intensive influence on human health and the aquati c ecological environment and need to be monitored critically.For the specific and highly sensitive analysis performance,agold-magnetic composite nanoparti clemodified by aptamer-cDNAfluorescent hybridization probe(Fe_(3)O_(4)@MIL-101-NH_(2)@Au@aptamer)was prepared and applied for sensing detection of MC-LR in water with laser-induced fluorescence(LIF).This work studied the feasibilit y,optimization of analysis conditions,specificity,stability of the method,an d sample analysis application.As a result,a high Brunauer-Emme tt-Teller(BET)specific surface area of 114.02 m 2·g^(-1) was achieved in Fe_(3)O_(4)@MIL-101-NH_(2)@AuNPs,which resulted in a high modification rate of up to 98.8%achieved for aptamer-cDNA fluorescenthybridization probe.With the excitation wavelength of 497 nm,the aptamer-cDNA fluorescent probe has a strong fluorescence response with the emission wavelength of 512 nm to the trace MC-LR.Under the optimal conditions(pH 7.5,NaCl concentration 500 mmol·L^(-1),nanogold size 20 nm,analytical time 30 min),a good linear relatio nship between MC-LR concentration and fluorescence intensity was achieved in a wide linear range(0.020~3.000μg·L^(-1))with the limit of detection(LO D)as low as 0.006μg·L^(-1),which was 1.6~22.3 folds better than that of the most fluorescence methods reported previously.The relative standard de viation(RSD)of intra-day,intra-day,and inter-batch was gained in 1.7%~8.8%,and the relative error(RE)of-4.3%~4.1%.High specific selec tivity and low cross-reactivity for MC-LR(1.0μg·L^(-1))were also achi eved using theas-prepared fluorescent probe,even if the concentration of inte rfering toxins(MC-RR,MC-YR,OA)was 100 folds higher than that of MC-LR.The fluorescence responses of MC-LR in these mixtures werewell consistent with that of MC-LR in the standard solution.Applied to the analysis of samples fr om the Minjiang River,Lake W
作者
齐国敏
童诗谦
林旭聪
QI Guo-min;TONG Shi-qian;LIN Xu-cong(College of Chemistry,Fuzhou University,Fuzhou 350108,China;Institute of Food Safety and Environment Monitoring,Fuzhou University,Fu zhou 350108,China)
出处
《光谱学与光谱分析》
SCIE
EI
CAS
CSCD
北大核心
2023年第12期3813-3819,共7页
Spectroscopy and Spectral Analysis
基金
国家重点研发计划课题(2018YFC1602902-3)
海洋服务与渔业高质量发展专项(FJHY-YYKJ-2023-1-1)资助。
