金纳米颗粒在玻碳电极表面的固载及其对抗坏血酸的电催化氧化
Immobilization of Gold Nanoparticles on the Surface of Glassy Carbon Electrode and Electrocatalytic Oxidation of Ascorbic Acid at the Electrode
摘 要
采用电化学方法先在玻碳电极(GCE)表面共价键合一末端带有巯基的2-氨基乙硫醇(AET)单层,通过硫-金相互作用将金纳米颗粒(GNP)固载在玻碳电极表面,制备了GNP修饰的GNP-AET/GCE电极.采用X射线光电子能谱和循环伏安法对固载纳米金的玻碳电极的结构和性能进行表征.研究发现:GNP-AET/GCE电极不仅对抗坏血酸具有良好的催化性能,使其氧化过电位由玻碳电极上的0.53 V负移到0.33 V,氧化峰电流明显增加,而且能将多巴胺和抗坏血酸在玻碳电极上重叠的氧化波分成两个独立的氧化峰,峰间电位差为0.29 V,提出了用差分脉冲伏安法在多巴胺共存在测定抗坏血酸的选择性方法.峰电流与抗坏血酸浓度在8.5×10-6~1.0×10-4mol·L-1之间呈线性关系,其检出限为4.7×10-6mol·L-1.
2-氨基乙硫醇
金纳米颗粒
多巴胺
抗坏血酸
Glassy carbon electrode
2-Aminoethanethiol
Gold nanoparticle
Dopamine
Ascorbic acid
Abstract
Gold nanoparticle (GNP) modified glassy carbon electrode (GCE) was prepared first by covalent-linking,through electrochemical method,a monolayer of 2-aminoethanethiol (AET) on the surface of GCE,and then through intereaction of gold with the mercapto group at the terminal of AET molecule,to immobilize GNP on the surface of the GCE.This modified electrode was named abbreviately as GNP-AET/GCE.The structure and property of the GNP-AET/GCE were characterized by X-ray photoelectron spectroscopy and cyclic voltammetry.It was found that GNP-AET/GCE showed not only effective catalytic property to ascorbic acid in making a negative shift of its oxidation potential from 0.53 V (at bare GCE) to 0.33 V and a remarkable increase in oxidation peak current,but also a clear separation of the originally overlapped oxidation waves of ascorbic acid and dopamine at the bare GCE into 2 separate oxidation peaks,between which the potential difference attained to a value of 0.29 V.Based on these findings,a selective method for determination of ascorbic acid in the presence of dopamine by differential pulse voltammetry was proposed.Linear relationship between values of peak current and concentration of ascorbic acid was obtained in the range of 8.5×10-6-1.0×10-4mol·L-1,with its detection limit of 4.7×10-6mol·L-1.
中图分类号 O657
所属栏目 试验与研究
基金项目 上海市教育委员会资助项目(No.05DZ16)
收稿日期 2007/7/2
修改稿日期
网络出版日期
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备注黄文华(1968-),男,河南永城人,讲师,主要研究方向为电分析化学.
引用该论文: HUANG Wen-hua,WANG Bai-mu,ZHANG Lei. Immobilization of Gold Nanoparticles on the Surface of Glassy Carbon Electrode and Electrocatalytic Oxidation of Ascorbic Acid at the Electrode[J]. Physical Testing and Chemical Analysis part B:Chemical Analysis, 2008, 44(4): 299～303
黄文华,王百木,张雷. 金纳米颗粒在玻碳电极表面的固载及其对抗坏血酸的电催化氧化[J]. 理化检验－化学分册, 2008, 44(4): 299～303
被引情况:
【1】李远刚,李华静,马小单,韦萍, "银纳米颗粒的合成及其与曙红Y的相互作用",理化检验－化学分册 47, 1001-1004(2011)
【2】王明艳,许兴友,马卫兴,曹志凌,许瑞波, "一阶微分线性扫描伏安法直接测定复方鱼腥草片中槲皮素",理化检验－化学分册 46, 1125-1128(2010)
【3】张钱丽,肖昕,张蓉,戴鹏,周帅,冯刚, "介孔碳/纳米金修饰电极同时测定多巴胺、抗坏血酸和尿酸",理化检验－化学分册 51, 1018-1022(2015)
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参考文献
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【3】Yu A,Chen H.Electrocatalytic oxidation and determination of ascorbic acid at poly (glutamic acid) chemically modified electrode[J].Anal Chim Acta,1997,344(3):181-185．
【4】Mo J W,Ogorevc B.Simultaneous measurement of dopamine and ascorbate at their physiological levels using voltammetric microprobe based on overoxidized poly (1,2-phenylenediamine)-coated carbon fibe[J].Anal Chem,2001,73(6):1196-1202．
【5】Raj C R,Tokuda K,Ohsaka T.Electroanalytical applications of cationic self-assembled monolayers: square-wave voltammetric determination of dopamine and ascorbate[J].Bioelectrochemistry,2001,53(2):183-191．
【6】Zhang L,Jia J,Zou X,et al.Simultaneous determination of dopamine and ascorbic acid at an in-site functionalized self-assembled monolayer on gold electrode[J].Electroanalysis,2004,16:1413-1418．
【7】Raj C R,Ohsaka T.Electroanalysis of ascorbate and dopamine at a gold electrode modified with a positively charged self-assembled monolayer[J].J Electroanal Chem,2001,496(1/2):44-49．
【8】Raj C R,Okajima T,Ohsaka T.Gold nanoparticle arrays for the voltammetric sensing of dopamine[J].J Electroanal Chem,2003,543(2):127-133．
【9】张雷,林祥钦.单分子层氨基丁酸共价修饰玻碳电极同时测定多巴胺、尿酸和抗坏血酸[J].高等学校化学学报,2003,24(4):591-594．
【10】Lin X,Zhang L.Simultaneous determination of dopamine and ascorbic acid at glutamic acid modified graphite electrode[J].Anal Lett,2001,34:1585-1601．
【11】Zhang L,Lin X.Covalent modification of glassy carbon electrodes with glycine for voltammetric separation of dopamine and ascorbic acid[J].Anal Bioanal Chem,2001,370:956-962．
【12】Zhang L,Lin X.Separation of anodic peaks of ascorbic acid and dopamine at an alanine covalently modified glassy carbon electrode[J].Analyst,2001,126:1760-1763．
【13】Frens G.Controlled nucleation for the regulation of the particle size in monodisperse gold suspensions[J].Nature Physical Science,1973,241(1):20-22．
【14】Barbier B,Pinson J,Desarmot G,et al.Electrochemical bonding of amines to carbon fiber surfaces toward improved carbon-epoxy composites[J].J Electrochem Soc,1990,137:1757-1764．
【15】Deinhammer R S,Mankit H,Anderegg J W,et al.Electrochemical oxidation of amine-containing compounds: a route to the surface modification of glassy carbon electrodes[J].Langmuir,1994,10(4):1306-1313．
【16】Cheng Q,Brajter-Toth A.Permselectivity,sensitivity,and amperometric pH sensing at thioctic acid monolayer microelectrodes[J].Anal Chem,1996,68(23):4180-4185．
【17】Dayton M A,Ewing A G,Wightman R M.Response of microvoltammetric electrodes to homogeneous catalytic and slow heterogeneous charge-transfer reactions[J].Anal Chem,1980,52(14):2392-2396．
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