Determination of Hg2+ by Fluorescence Quenching with PNTU Probe
摘 要
制备了一种硫脲分子PNTU探针,基于其对Hg2+的专一性比色识别,建立了荧光猝灭法测定Hg2+含量的方法。在4-溴-1,8-萘酐的乙醇溶液中,逐滴加入2 mL 80%(质量分数)水合肼溶液,反应完成后,经抽滤,乙醇、水洗涤后干燥,再加入10 mL吡咯烷,在氮气保护下继续反应,得到红褐色固体。将其溶于15 mL乙腈中,室温搅拌下滴加1 mL异硫氰酸苯酯,反应完成后,经减压浓缩、水洗得到PNTU探针。将PNTU探针溶液与体积比为8∶2的乙腈-4-羟乙基哌嗪乙磺酸缓冲液的混合液混匀,然后加入含Hg2+的样品溶液,采用荧光猝灭法测定体系的荧光强度。结果显示:当加入Hg2+时,体系的荧光强度明显降低,溶液颜色由黄色变成橙红色;干扰试验表明PNTU探针在有其他金属离子存在的情况下仍可检测出Hg2+;Hg2+浓度在20.0 μmol·L-1以内与其对应体系的荧光强度降低值呈线性关系,检出限(3S/N)为1.8 nmol·L-1;对实际水样进行3个浓度水平的加标回收试验,Hg2+的回收率为99.6%~104%,测定值的相对标准偏差(n=5)为0.85%~2.6%。基于PNTU探针制备了Hg2+的检测试纸,可方便快捷地检测样品中是否存在Hg2+。
Abstract
Based on specific colorimetric recognition of Hg2+ with PNTU probe, a method for the determination of Hg2+ by fluorescence quenching was established. In the ethanol solution of 4-bromo-1,8-naphthalene anhydride, 2 mL of 80% (mass fraction) hydrazine hydrate solution was added dropwise. After filtering, washing with ethanol and water and drying, pyrrolithane of 10 mL was added. Then reaction was running under the protection of nitrogen to give reddish-brown solid. The reddish-brown solid was dissolved in 15 mL of acetonitrile, and 1 mL of phenyl isothiocyanate was added by stirring at room temperature. After the reaction was completed, the PNTU probe was obtained after vacuum concentration and washing with water. PNTU probe solution was evenly mixed with a mixture of acetonitrile-4-hydroxyethyl piperazine ethanesulfonic acid buffer solution at volume ratio of 8∶2, then Hg2+ sample soution was added, and fluorescence intensity of the system was measured by fluorescence quenching. The results showed that the fluorescence intensity of PNTU system decreased obviously when Hg2+ was added, following color of the solution changed from yellow to orange-red, and the PNTU probe could detect Hg2+ in the presence of other metal ions. Linear relationship between concentration of Hg2+ and magnitude of decrease in fluorescence intensity of the system was kept within 20.0 μmol·L-1, with detection limit (3S/N) of 1.8 nmol·L-1. Recovery test was made by standard addition method on actual water samples at 3 concentration levels, giving results in the range of 99.6%-104%, and RSDs (n=5) of the determined values ranged from 0.85% to 2.6%. Detection strips based on PNTU probe were prepared, which could easily and quickly detect whether Hg2+ exists in the sample.
中图分类号 O657.3 DOI 10.11973/lhjy-hx202108002
所属栏目 试验与研究
基金项目 四川省科技厅资助项目(2018JY0299);四川省达州市科技局项目(20YYJC0001);四川省特色植物开发与研究重点实验室项目(TSZW2009);四川文理学院水处理研究专项(2018SCL005Y)
收稿日期 2020/7/23
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备注刘丹,副教授,硕士,主要从事有机小分子的合成及分子识别研究工作,601747850@qq.com
引用该论文: LIU Dan,CHEN Anyin,XIANG Wenjun,YAN Shuang,YANG Xiong. Determination of Hg2+ by Fluorescence Quenching with PNTU Probe[J]. Physical Testing and Chemical Analysis part B:Chemical Analysis, 2021, 57(8): 682~687
刘丹,陈安银,向文军,颜爽,杨雄. PNTU探针-荧光猝灭法测定Hg2+的含量[J]. 理化检验-化学分册, 2021, 57(8): 682~687
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【2】CUI X, ZHU L, WU J, et al. A fluorescent biosensor based on carbon dots-labeled oligodeoxyribonucleotide and graphene oxide for mercury(Ⅱ) detection[J]. Biosensors and Bioelectronics, 2015,63:506-512.
【3】HUANG P J J, WANG F, LIU J W. Cleavable molecular beacon for Hg2+ detection based on phosphorothioate RNA modifications[J]. Analytical Chemistry, 2015,87(13):6890-6895.
【4】DA SILVA M J, PAIM A P S, PIMENTEL M F, et al. Determination of mercury in rice by cold vapor atomic fluorescence spectrometry after microwave-assisted digestion[J]. Analytica Chimica Acta, 2010,667(1/2):43-48.
【5】CHEN L Y, OU C M, CHEN W Y, et al. Synthesis of photoluminescent Au ND-PNIPAM hybrid microgel for the detection of Hg2+[J]. ACS Applied Materials and Interfaces, 2013,5(10):4383-4388.
【6】HSU I H, HSU T C, SUN Y C. Gold-nanoparticle-based graphite furnace atomic absorption spectrometry amplification and magnetic separation method for sensitive detection of mercuric ions[J]. Biosensors and Bioelectronics, 2011,26(11):4605-4609.
【7】CHEN F Y, JIANG S J. Slurry sampling flow injection chemical vapor generation inductively coupled plasma mass spectrometry for the determination of As, Cd, and Hg in cereals[J]. Journal of Agricultural and Food Chemistry, 2009,57(15):6564-6569.
【8】HUSSAIN M M, RAHMAN M M, ARSHAD M N, et al. Hg2+ sensor development based on (E)-N'-nitrobenzylidene-benzenesulfonohydrazide (NBBSH) derivatives fabricated on a glassy carbon electrode with a nafion matrix[J]. ACS Omega, 2017,2(2):420-431.
【9】KHATUA S, SCHMITTEL M. A single molecular light-up sensor for quantification of Hg2+ and Ag+ in aqueous medium: High selectivity toward Hg2+ over Ag+ in a mixture[J]. Organic Letters, 2013,15(17):4422-4425.
【10】黄小梅,邓祥.新型荧光碳点的制备及其在Hg2+检测中的应用[J].应用化学, 2019,36(5):603-610.
【11】李静雅,张爱菊,张小林.罗丹明B荧光猝灭法测定消毒液中过氧乙酸的含量[J].理化检验-化学分册, 2019,55(10):1194-1197.
【12】LIN W C, WU C Y, LIU Z H, et al. A new selective colorimetric and fluorescent sensor for Hg2+ and Cu2+ based on a thiourea featuring a pyrene unit[J]. Talanta, 2010,81(4/5):1209-1215.
【13】ZHANG Y M, SHI B B, ZHANG P, et al. A highly selective dual-channel Hg2+ chemosensor based on an easy to prepare double naphthalene Schiff base[J]. Science China Chemistry, 2013,56(5):612-618.
【14】AGARWALLA H, MAHAJAN P S, SAHU D, et al. A switch-on NIR probe for specific detection of Hg2+ ion in aqueous medium and in mitochondria[J]. Inorganic Chemistry, 2016,55(22):12052-12060.
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