磁性碲化镉掺杂荧光传感器的分子动力学模拟、合成及其检测对硝基苯酚的应用研究

详细信息    查看全文 | 推荐本文 |

英文篇名：Molecular Dynamics Simulation,Synthesis and Detection of 4-Nitrophenol Fluorescence Sensor by Hybrid Magnetic Cadmium Telluride 作者：徐婉珍 ; 邱春孝 ; 黄卫红 ; 闫永胜 ; 刘鸿 ; 杨文明 英文作者：XU Wan-Zhen;QIU Chun-Xiao;HUANG Wei-Hong;YAN Yong-Sheng;LIU Hong;YANG Wen-Ming;School of the Environment and Safety Engineering,Jiangsu University;School of Materials Science and Engineering,Jiangsu University;School of Chemistry and Chemical Engineering,Jiangsu University;Institute of Theoretical Chemistry,Laboratory of Theoretical and Computational Chemistry,Jilin University; 关键词：磁性量子点 ; 分子印迹聚合物 ; 对硝基苯酚 ; 分子动力学模拟 英文关键词：Magnetic quantum dots;;Molecular imprinted polymers;;4-Nitrophenol;;Molecular dynamics simulation 中文刊名：FXHX 英文刊名：Chinese Journal of Analytical Chemistry 机构：江苏大学环境与安全工程学院;江苏大学材料科学与工程学院;江苏大学化学化工学院;吉林大学理论化学研究所理论化学计算实验室; 出版日期：2018-08-13 出版单位：分析化学 年：2018 期：v.46 基金：国家自然科学基金项目(No.21677064);; 江苏省自然科学基金项目(Nos.BK20151323,BK20151337)资助~~ 语种：中文; 页：FXHX201808013 页数：9 CN：08 ISSN：22-1125/O6 分类号：71-79

摘要

基于COMPASS力场,建立25组对硝基苯酚(4-NP)、3-氨丙基三乙氧基硅烷(APTES)和正硅酸四乙酯(TEOS)的预聚合体系,运用分子动力学方法进行计算模拟。利用径向分布函数及积分数据,筛选出体系4-NP∶APTES∶TEOS的最佳配比为10∶20∶80。实验中,采用水热法合成磁性纳米颗粒,在其表面修饰氨基,与巯基乙酸修饰的碲化镉量子点结合,形成基于硅基表面的磁性量子点。根据分子动力学模拟的结果,以4-NP为模板分子、APTES为功能单体、TEOS为交联剂,按照计算机模拟的配比,在磁性量子点表面合成4-NP分子印迹聚合物,并将其作为传感器的识别元件,成功应用于检测水环境中的4-NP,方法的线性检测范围为5~150 ng/mL,检出限为1 ng/mL,回收率为98.7%~101.2%,相对标准偏差为1.5%~2.4%。
        Twenty five molecular imprinting prepolymerization systems were performed based on COMPASS force field to optimize the imprinting shell of the fluorescent sensor. The result revealed that the optimum mole ratio of 4-Nitrophenol( 4-NP),3-aminopropyltriethoxysilane( APTES) and tetraethylorthosilicate( TEOS) in this system was 10 ∶ 20 ∶ 80,which was the most stable between template and functional monomer cluster.Uniform magnetite nanaocrystals prepared by hydrothermal method were subsequently embedded in the spherical silica using the reverse microemulsion polymerization. The magnetic silica microspheres were modified with amide groups to adsorb the mercaptoacetic acid capped Cd Te nanocrystals. Finally,according to the results of molecular dynamics simulation, the imprinting shell was anchored on the multifunctional nanocomposites. Under the optimal conditions,a linear relationship between relative fluorescence intensity and concentration of 4-NP was obtained covering the concentration range from 5 to 150 ng/mL with a limit of detection of 1 ng/ml. The feasibility of the fluorescent sensor was successfully evaluated through the analysis of 4-NP in river water. The recoveries were from 98.7% to 101.2%,and the relative standard deviation ranged from 1.5% to 2.4%.

引文

1 Lai B,Zhang Y H,Chen Z Y,Yang P,Zhou Y X,Wang J L.Appl.Catal.B,2014,144:816-830
    2 Zhang B,Li F,Wu T,Sun D J,Li Y J.Colloids Surfaces A,2015,464:78-88
    3 Ghosh S.Tetrahedron Lett.,2015,56:6738-6741
    4 Zhang Y H,Zhang C,Dong F L,Chen M M,Cao J C,Wang H Y,Jiang M.Regul.Toxicol.Pharmacol.,2017,87:88-94
    5 Nasrollahzadeh M,Sajadi S M,Rostami-Vartooni A,Bagherzadeh M,Safari R.J.Mol.Catal.A,2015,400:22-30
    6 Keith L H,Telliard W A.Environ.Sci.Technol.,1979,13:416-423
    7 Wu P G,Zhang L Q,Yang D J,Zhang J,Hu Z Y,Wang L Y,Ma B J.J.Sep.Sci.,2016,39(5):904-909
    8 Czech T,Bonilla N B,Gambus F,González R R,Marín-Sez J,Vidal J L M,Frenich A G.Sci.Total Environ.,2016,557:681-687
    9 Nezamzadeh-Ejhieh A,Khorsandi S.J.Ind.Eng.Chem.,2014,20(3):937-946
    10 Wang J H,Ren L,Jia Y,Ruth N,Shi Y H,Qiao C,Yan Y C.Toxicol.Environ.Chem.,2016,98(2):226-240
    11 Xu S F,Lu H Z.Biosens.Bioelectron.,2015,73:160-166
    12 Sun B H,Ni X J,Cao Y H,Cao G Q.Biosens.Bioelectron.,2017,91:354-358
    13 Tretjakov A,Syritski V,Reut J,Boroznjak R,pik A.Anal.Chim.Acta,2016,902:182-188
    14 ZHANG Tao-Na,XU Xue-Wen,DONG Liang,TAN Zhao-Yi,LIU Chun-Li.Acta Physico-Chimica Sin.,2017,33:2013-2021张陶娜,徐雪雯,董亮,谭昭怡,刘春立.物理化学学报,2017,33:2013-2021
    15 WANG Zi-Min,ZHENG Mo,XIE Yong-Bing,LI Xiao-Xia,ZENG Ming,CAO Hong-Bing,GUO Li.Acta Physico-Chimica Sin.,2017,33(7):1399-1410王子民,郑默,谢勇冰,李晓霞,曾鸣,曹宏斌,郭力.物理化学学报,2017,33(7):1399-1410
    16 XIE Wei,XU Ze-Ren,WANG Ming,XU Si-Chuan.Acta Physico-Chimica Sin.,2016,32:907-920谢炜,徐泽人,王明,徐四川.物理化学学报,2016,32:907-920
    17 CAO Liao-Ran,ZHANG Chun-Yu,ZHANG Ding-Lin,CHU Hui-Ying,ZHANG Yue-Bin,LI Guo-Hui.Acta Physico-Chimica Sin.,2017,33:1354-1365曹了然,张春煜,张鼎林,楚慧郢,张跃斌,李国辉.物理化学学报,2017,33:1354-1365
    18 YANG Zhen,LIU Hai,HE Yuan Hang.Acta Physico-Chimica Sin.,2016,32:1977-1982杨镇,刘海,何远航.物理化学学报,2016,32:1977-1982
    19 WANG Yun-He,QIN Yuan,YAO Man,WANG Xu-Dong,LI Shu-Ying,WANG Dong,CHEN Ting.Acta Physico-Chimica Sin.,2016,32:2255-2263王云赫,秦圆,姚曼,王旭东,李淑颖,王栋,陈婷.物理化学学报,2016,32:2255-2263
    20 Shoravi S,Olsson G D,Karlsson B C G,Nicholls I A.Int.J.Mol.Sci.,2010,15:10622-0634
    21 Meier F,Schott B,Riedel D,Mizaikoff B.Anal.Chim.Acta,2012,744:68-74
    22 Nicholls I A,Andersson H S,Golker K,Henschel H,Karlsson B C G,Olsson G D,Rosengren A M,Shoravi S,Suriyanarayanan S,Wiklander J G,Wikman S.Anal.Bioanal.Chem.,2011,400:1771-1786
    23 Sun H.J.Phys.Chem.B,1998,5647:7338-7364
    24 Sun H,Ren P,Fried J R.Comput.Theor.Polym.Sci.,1998,8:229-246