Fe_3O_4磁性纳米粒子催化动力学荧光法测定微量过氧化氢
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摘要
Fe3O4磁性纳米粒子(Fe3O4MNPs)具有模拟过氧化氢酶的催化特性。基于Fe3O4MNPs催化H2O2氧化吡罗红建立了催化动力学荧光法测定H2O2的方法。对Fe3O4MNPs-吡罗红-H2O2体系的荧光光谱进行了研究,并考查了一些因素对体系的影响。所研究的催化反应分别在7~13min和13~18min内为假零级反应,对应的表观速率常数分别为1.33×10-1s-1和8.41×10-2s-1。反应时间为18 min时,催化反应的表观活化能为40.42 k J·mol-1。在最佳实验条件下,方法的线性范围为3.20×10-4~1.12×10-2mol·L-1,检出限为1.65×10-4mol·L-1。该法可用于消毒液、雨水、自来水及合成样品中H2O2含量的测定。
Fe3O4magnetic nanomaterials exhibit an intrinsic peroxidase-like catalytic activity. A new kinetic spectrofluorimetric method was developed for the determination of H2O2 based on the catalytic activity of Fe3O4 MNPs for the oxidation of pyronine by H2O2. The characteristic spectra of fluorescence of the system were discussed. The effects of some experiments conditions were investigated. The catalytic reaction were considered as pseudozero order in 7 ~ 13 min and 13 ~ 18 min,respectively,and the corresponding apparent rate constants were 1. 33×10-1s-1and 8. 41×10-2s-1. When the reacting time was taken as 18 min,the apparent activity energy of the catalytic reaction was found to be 40. 42 k J·mol-1. Under the optimum conditions,the linear range of H2O2 was 3. 20×10-4~ 1. 12 ×10-2mol·L-1with the limit of detection 1. 65×10-4mol·L-1. This method was suitable for the determination of hydrogen peroxide in disinfector,rain water,tap water and synthetic samples.
Fe3O4magnetic nanomaterials exhibit an intrinsic peroxidase-like catalytic activity. A new kinetic spectrofluorimetric method was developed for the determination of H2O2 based on the catalytic activity of Fe3O4 MNPs for the oxidation of pyronine by H2O2. The characteristic spectra of fluorescence of the system were discussed. The effects of some experiments conditions were investigated. The catalytic reaction were considered as pseudozero order in 7 ~ 13 min and 13 ~ 18 min,respectively,and the corresponding apparent rate constants were 1. 33×10-1s-1and 8. 41×10-2s-1. When the reacting time was taken as 18 min,the apparent activity energy of the catalytic reaction was found to be 40. 42 k J·mol-1. Under the optimum conditions,the linear range of H2O2 was 3. 20×10-4~ 1. 12 ×10-2mol·L-1with the limit of detection 1. 65×10-4mol·L-1. This method was suitable for the determination of hydrogen peroxide in disinfector,rain water,tap water and synthetic samples.
引文
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[5]Lv G,He F,Wang X M,et al.Novel nanocomposite of nano Fe3O4and polylactide nanofibers for application in drug uptake and induction of cell death of leukemia cancer cells[J].Langmuir,2008,24(5):2151-2156.
[6]Yang H H,Zhang S Q,Chen X L,et al.Magnetite-containing spherical silica nanoparticles for biocatalysis and bioseparations[J].Anal Chem,2004,76(5):1316-1321.
[7]Gao L Z,Zhuang J,Nie L,et al.Intrinsic peroxidase-like activity of ferromagnetic nanoparticles[J].Nat Nanotech,2007,2(9):577-583.
[8]Wei H,Wang E K.Fe3O4magnetic nanoparticles as peroxidase mimetics and their applications in H2O2and glucose detection[J].Anal Chem,2008,80(6):2250-2254.
[9]Chang Q,Deng K J,Zhu L H,et al.Determination of hydrogen peroxide with the aid of peroxidase-like Fe3O4magnetic nanoparticles as the catalyst[J].Microchim Acta,2009,165(3-4):299-305.
[10]Jiang Z L,Kun L,Ouyang H X,et al.A Simple and sensitive fluorescence quenching method for the determination of H2O2using rhodamine B and Fe3O4nanocatalyst[J].J Fluoresc,2011,21(5):2015-2020.
[11]Jiao X,Song H J,Zhao H H,et al.Well-redispersed ceria nanoparticles:Promising peroxidase mimetics for H2O2and glucose detection[J].Anal Methods,2012,4(10):3261-3267.
[12]Luo W,Abbas M E,Zhu L H,et al.Rapid quantitative determination of hydrogen peroxide by oxidation decolorization of methyl orange using a Fenton reaction system[J].Anal Chim Acta,2008,629(1-2):1-5.
[13]Nakahara R,Kashitani S,Hayakawa K,et al.Fluorophotometric determination of hydrogen peroxide with fluorescin in the presence of cobalt(II)and reaction against other reactive oxygen species[J].J Fluoresc,2009,19(5):769-775.
[14]Yang X Y,Guo Y S,Mei Z H.Chemiluminescent determination of H2O2using 4-(1,2,4-triazol-1-yl)phenol as an enhancer based on the immobilization of horseradish peroxidase onto magnetic beads[J].Anal Biochem,2009,393(1):56-61.
[15]Liu X H,Bu C H,Nan Z H,et al.Enzymes immobilized on amine-terminated ionic liquid-functionalized carbon nanotube for hydrogen peroxide determination[J].Talanta,2013,105(15):63-68.
[16]Xia P P,Liu H Q,Tian Y.Cathodic detection of H2O2based on nanopyramidal gold surface with enhanced electron transfer of myoglobin[J].Biosens and Bioelectron,2009,24(8):2470-2474.
[17]Hou C T,Xu Q,Yin L N,et al.Meta-organic framework templated synthesis of Co3O4 nanoparticles for direct glucose and H2O2detection[J].Analyst,2012,137(24):5803-5808.
[18]武汉大学.分析化学(第五版),上册[M].北京:高等教育出版社,2005:242.
[19]Wang N,Zhu L H,Wang D L,et al.Sono-assisted preparation of highly-efficient peroxidase-like Fe3O4magnetic nanoparticles for catalytic removal of organic pollutants with H2O2[J].Ultrason Sonochem,2010,17(3):526-533.