石墨烯-纳米银修饰电极检测过氧化氢
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摘要
以氧化石墨烯(GO)和硝酸银为原料,通过共合成法,制备了还原氧化石墨烯负载纳米银颗粒(AgNPs-rGO)复合物,并将AgNPs-rGO复合物修饰在碳糊电极(CPE)上,制得AgNPs-rGO/CPE电极。通过XRD、SEM和EDS技术对AgNPs-rGO的结构进行了表征与测试。结果表明,AgNPs很好地负载在了rGO上,且银元素的质量分数高达50.57%。当硝酸银浓度为0.02 mol/L时,AgNPs-rGO/CPE电极表现出最佳的电化学性能。在pH=5.5的磷酸盐缓冲溶液中,对过氧化氢在AgNPs-rGO/CPE电极上的电化学行为进行了考察。结果表明,AgNPs-rGO/CPE对过氧化氢的电化学检测表现出良好的稳定性,相对标准偏差仅为3.7%。当过氧化氢的浓度在1.0×10~(-8)~1.0×10~(-6)mol/L范围内时,过氧化氢的响应电流值ΔI与其浓度对数lgc呈现良好的线性关系,线性相关系数R~2高达0.993 4。将其应用于自来水样品中的过氧化氢检测,得到的加标回收率达到97.1%,多次重复检测的相对标准偏差仅为4.7%,表明制备的AgNPs-rGO/CPE对过氧化氢的电化学检测具有良好的重现性和稳定性。
Silver nanoparticles( AgNPs)-reduced graphene oxide( AgNPs-rGO) composite was prepared by co-synthesized,and then it was introduced into carbon paste electrode( CPE) to prepare AgNPs-rGO/CPE electrode. The resulting AgNPs-rGO composite was characterized by XRD,SEM and EDS. The results indicated AgNPs was well loaded on rGO and the mass fraction of silver element was up to 50. 57%. When the amount of silver nitrate was 0. 02 mol/L,the AgNPs-rGO/CPE electrode showed the best electrochemical performance. The electrochemical behavior of hydrogen peroxide at AgNPs-rGO/CPE electrode was investigated in pH = 5. 5 phosphate buffer solution. As a result,this electrode exhibited a good stability for the electrochemical determination of hydrogen peroxide with a relative standard deviation( RSD) of 3. 7%.When the concentration of hydrogen peroxide was within the range of 1.0 × 10~(-8)~ 1. 0 × 10~(-6)mol/L,the electrochemical current of hydrogen peroxide increased linearly with the concentration of hydrogen peroxide( R~2= 0. 9934). The electrode for the detection of hydrogen peroxide in drinking water was developed. The recovery rate and RSD in drinking water sample were 97. 1% and 4. 7%,respectively. The results revealed that the prepared AgNPs-rGO/CPE electrode could be used for electrochemical detection of hydrogen peroxide with excellent reproducibility and stability.
Silver nanoparticles( AgNPs)-reduced graphene oxide( AgNPs-rGO) composite was prepared by co-synthesized,and then it was introduced into carbon paste electrode( CPE) to prepare AgNPs-rGO/CPE electrode. The resulting AgNPs-rGO composite was characterized by XRD,SEM and EDS. The results indicated AgNPs was well loaded on rGO and the mass fraction of silver element was up to 50. 57%. When the amount of silver nitrate was 0. 02 mol/L,the AgNPs-rGO/CPE electrode showed the best electrochemical performance. The electrochemical behavior of hydrogen peroxide at AgNPs-rGO/CPE electrode was investigated in pH = 5. 5 phosphate buffer solution. As a result,this electrode exhibited a good stability for the electrochemical determination of hydrogen peroxide with a relative standard deviation( RSD) of 3. 7%.When the concentration of hydrogen peroxide was within the range of 1.0 × 10~(-8)~ 1. 0 × 10~(-6)mol/L,the electrochemical current of hydrogen peroxide increased linearly with the concentration of hydrogen peroxide( R~2= 0. 9934). The electrode for the detection of hydrogen peroxide in drinking water was developed. The recovery rate and RSD in drinking water sample were 97. 1% and 4. 7%,respectively. The results revealed that the prepared AgNPs-rGO/CPE electrode could be used for electrochemical detection of hydrogen peroxide with excellent reproducibility and stability.
引文
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[3]Chen W,Cai S,Ren Q,et al.Recent advances in electrochemical sensing for hydrogen peroxide:a review[J].Analyst,2012,137(1),49-58.
[4]Kiba N,Tokizawa T,Kato S J,et al.Flow-through micro sensor using immobilized peroxidase with chemiluminometric FIA system for determining hydrogen peroxide[J].Analytical Sciences,2003,19(6):823-827.
[5]Zhang L,Wong G.Optimal conditions and sample storage for the determination of H2O2in marine waters by the scopoletinhorseradish peroxidase fluorometric method[J].Talanta,1999,48(5):1031-1038.
[6]Fan Huafeng(范华峰),Zhang Zhongyi(张忠义),Liu Zhenlin(刘振林).Spectrophotometric determination of hydrogen peroxide in food[J].Chinese Journal of Health laboratory Technology(中国卫生检验杂志),2006,16(9):1079-1080.
[7]Deng Zifeng(邓子峰),Zhang Hongwei(张洪伟),Jiao Yuzhu(焦玉珠).Hydrogen peroxide biosensor based on cytochrome C/Zinc Oxide[J].Chinese Journal of Analytical Chemistry(分析化学),2007,35(7):1011-1014.
[8]Wang L,Wang E.A novel hydrogen peroxide sensor based on horseradish peroxidase immobilized on colloidal Au modified ITO electrode[J].Electrochemistry Communication,2004,6(2):225-229.
[9]Song M,Hwang S,Whang D.Non-enzymatic electrochemical Cu O nanoflowers sensor for hydrogen peroxide detection[J].Talanta,2010,5(80):1648-1652.
[10]Ye Wenyu(叶文玉),Zhang Fute(张付特),Lu Peizhong(路培中),et al.Preparation and tribological properties of surface modified Ag nanoparticles[J].Fine Chemicals(精细化工),2007,24(9):863-866.
[11]Wu Fengci(吴凤慈),Liu Dongzhi(刘东志),Zhou Xueqin(周雪琴),et al.Green synthesis of amino acid functionalized silver nanoparticles and their conductivity[J].Fine Chemicals(精细化工),2015,32(9):980-984.
[12]Yadav D K,Gupta R,Ganesan V,et al.Electrochemical sensing platform for hydrogen peroxide determination at low reduction potential using silver nanoparticle-incorporated bentonite clay[J].Journal of Applied Electrochemistry,2016,46(1):103-112.
[13]Yin Y,Shen M,Tan Z,et al.Particle coating-dependent interaction of molecular weight fractionated natural organic matter:impacts on the aggregation of silver nanoparticles[J].Environmentalence&Technology,2015,49(11):6581-6589.
[14]Duan S,Rui Y,Huang Y.Polyethylenimine-carbon nanotubes composite as an electrochemical sensing platform for silver nanoparticles[J].Talanta,2016,160:607-613.
[15]Cloake S J,Toh H S,Lee P T,et al.Anodic stripping voltammetry of silver nanoparticles:aggregation leads to incomplete stripping[J].Chemistry Open,2015,4(1):22-26.
[16]Allen M,Tung V,Kaner R.Honeycomb carbon:a review of graphene[J].Chemical Review,2009,110(1):132-145.
[17]Stankovich S,Dikin D,Dommett G,et al.Graphenebased composite materials[J].Nature,2006,442(7100):282-286.
[18]Gomez-Navarro C,Weitz R,Kern K.Electronic transport properties of individual chemically reduced graphene oxide sheets[J].Nano Letter,2007,7(11):3499-3503.
[19]Chen Y,Zhu Q,Tsumori N,et al.Immobilizing highly catalytically active noble metal nanoparticles on reduced graphene oxide:A non-noble metal sacrificial approach[J].Journal of the American Chemical Society,2015,137(1):106-109.
[20]Marcano D C,Kosynkin D V,Berlin J M,et al.Improved synthesis of graphene oxide[J].ACS nano,2010,4(8):4806-4814.
[21]Khan M E,Khan M M,Cho M H.Biogenic synthesis of a Aggraphene nanocomposite with efficient photocatalytic degradation,electrical conductivity and photoelectrochemical performance[J].New Journal of Chemistry,2015,39(10):8121-8129.
[22]Wei Y,Zuo X,Li X,et al.Dry plasma synthesis of graphene oxide-Ag nanocomposites:A simple and green approach[J].Materials Research Bulletin,2014,53:145-150.
[23]Zhu Ling(朱玲).Discussion on the content determination of the commercial product-hydrogen peroxide[J].Anhui Chemical Industry(安徽化工),2002,(6):45-46.