铜修饰多孔镍自支撑电极的构建及其葡萄糖氧化性能

doi:10.11944/j.issn.1000-0518.2019.09.190005

摘要/Abstract

摘要：

采用水热合成法制备了正八面体Cu₂O/Cu修饰的多孔Ni(NF)自支撑电极(Cu₂O/Cu-NF),并对其进行了形貌和结构表征。在三电极体系下,在碱性介质中以循环伏安法和恒电位安培法测试其对葡萄糖催化氧化性能。结果表明,150 ℃水热法制备的自支撑电极对葡萄糖的电催化氧化活性最强。响应电流与葡萄糖浓度在3.7×10^-3~1.1 mmol/L和1.4~5.0 mmol/L范围内呈线性相关,响应灵敏度分别是6929和706.1 μA/(mmol·L^-1·cm²),且具有良好的选择性和稳定性,对无酶葡萄糖传感器的发展有重要意义。

关键词: 电催化, 葡萄糖氧化, 多孔Ni自支撑电极

Abstract:

Porous Ni(nickel foam, NF) self-supported electrodes modified by Cu₂O/Cu were fabricated by hydrothermal method. Their morphology and structure were characterized by X-ray diffraction(XRD) and field-emission scanning electron microscopy(FESEM). The resulted surface of porous Ni is completely covered with octahedral Cu₂O/Cu composites of different sizes. The maximum diameter of the octahedron is about 5 μm. The glucose catalytic oxidation activity of Cu₂O/Cu-NF was measured by cyclic voltammetry and constant potential amperometric method in alkaline medium with three-electrode system. The results show that the Cu₂O/Cu-NF fabricated at 150 ℃ has the strongest electrocatalytic activity. The linear relationship of response current and glucose concentration could be observed clearly in the range of 3.7×10^-3~1.1 mmol/L and 1.4~5.0 mmol/L, with sensitivity of 6929 μA/(mmol·L^-1·cm²) and 706.1 μA/(mmol·L^-1·cm²), respectively. Satisfyingly, the Cu₂O/Cu-NF electrode is successfully employed to eliminate the interferences from uric acid(UA), acid ascorbic(AA) and L-proline(L-P) during the catalytic oxidation of glucose. The response current of Cu₂O/Cu-NF electrode for glucose electrocatalytic oxidation could reach 91.6% of the original current after one month. The Cu₂O/Cu-NF electrode allows highly sensitive, excellently selective, stable, and fast amperometric sensing of glucose and thus is promising for the future development of nonenzymatic glucose sensors.

Key words: electrocatalysis, glucose oxidation, porous Ni self-supported electrode

车婷华, 谭潇, 晏嘉伟, 宋凤丹, 张红梅, 齐随涛. 铜修饰多孔镍自支撑电极的构建及其葡萄糖氧化性能[J]. 应用化学, 2019, 36(9): 1091-1098.

CHE Tinghua, TAN Xiao, YAN Jiawei, SONG Fengdan, ZHANG Hongmei, QI Suitao. Synthesis of Copper Modified Porous Nickel Self-supported Electrode and Its Catalytic Oxidation of Glucose[J]. Chinese Journal of Applied Chemistry, 2019, 36(9): 1091-1098.

参考文献

[1]	Brouzgou A,Tsiakaras P.Electrocatalysts for Glucose Electrooxidation Reaction:A Review[J]. Top Catal,2015,58(18):1-17.
[2]	BAI Hongyan,WANG Xiuhua,DAI Zhihui,et al. Research Development of Non-enzymatic Glucose Detection[J]. Chinese J Appl Chem,2012,29(6):611-615(in Chinese). 白红艳,王秀华,戴志晖. 无酶葡萄糖检测的研究进展[J]. 应用化学,2012,29(6):611-615.
[3]	Wang G F,He X P,Wang L L,et al. Non-enzymatic Electrochemical Sensing of Glucose[J]. Microchim Acta,2013,180(3):161-186.
[4]	Su S,Lu Z W,Li J,et al. MoS2-Au@Pt Nanohybrid as a Sensing Platform for Electrochemical Nonenzymatic Glucose Detection[J]. New J Chem,2018,42(9):6750-6755.
[5]	Ma L,Wang X Y,Zhang Q R,et al. Pt Catalyzed Formation of a Ni@Pt/reduced Graphene Oxide Nanocomposite:Preparation and Electrochemical Sensing Application for Glucose Detection[J]. Anal Methods,2018,10(31):3845-3850.
[6]	Meg as-Sayago C,Bobadilla L F,Ivanova S,et al. Gold Catalyst Recycling Study in Base-free Glucose Oxidation Reaction[J]. Catal Today,2017,301:72-77.
[7]	Derrien E,Mounguenguidiallo M,Perret N,et al. Aerobic Oxidation of Glucose to Glucaric Acid under Alkaline-Free Conditions:Au-Based Bimetallic Catalysts and Effect of Residues in a Hemicellulose Hydrolysate[J]. Ind Eng Chem Res,2017,56(45):13176-13190.
[8]	Li F,Feng Y,Yang L M,et al. A Selective Novel Non-enzyme Glucose Amperometric Biosensor Based on Lectin Sugar Binding on Thionine Modified Electrode[J]. Biosens Bioelectron,2011,26(5):2489-2494.
[9]	Gough D A,Anderson F L,Giner J,et al. Effect of Coreactants on Electrochemical Glucose Oxidation[J]. Anal Chem,1978,50(7):941-944.
[10]	Vassilyev Y B,Khazova O A,Nikolaeva N N J. Kinetics and Mechanism of Glucose Electrooxidation on Different Electrode-Catalysts:Part I.Adsorption and Oxidation on Platinum[J]. Electroanal Chem,1985,196(1):105-125.
[11]	Guo C Y,Huo H H,Han X,et al. Ni/CdS Bifunctional Ti@TiO2 Core Shell Nanowire Electrode for High-Performance Nonenzymatic Glucose Sensing[J]. Anal Chem,2014,86(1):876-883.
[12]	Darvishi S,Souissi M,Kharaziha M,et al. Gelatin Methacryloyl Hydrogel for Glucose Biosensing Using Ni Nanoparticles-Reduced Graphene Oxide:An Experimental and Modeling Study[J]. Electrochim Acta,2018,261:275-283.
[13]	Zhang Q,Luo Q,Qin Z B,et al. Self-assembly of Graphene-Encapsulated Cu Composites for Nonenzymatic Glucose Sensing[J]. ACS Omega,2018,3(3):3420-3428.
[14]	Zhang Y,Zhao D Y,Zhu W X,et al. Engineering Multi-stage Nickel Oxide Rod-On-Sheet Nanoarrays on Ni Foam:A Superior Catalytic Electrode for Ultrahigh-Performance Electrochemical Sensing of Glucos[J]. Sens Actuators B,2018,255:416-423.
[15]	El-Refaei S M,Saleh M M,Awad M I. Enhanced Glucose Electrooxidation at a Binary Catalyst of Manganese and Nickel Oxides Modified Glassy Carbon Electrode[J]. J Power Sources,2013,223:125-128.
[16]	Amaniampong P N,Trinh Q T,Li K X,et al. Porous Structured CuO-CeO2 Nanospheres for the Direct Oxidation of Cellobiose and Glucose to Gluconic Acid[J]. Catal Today,2018,306:172-182.
[17]	Xu D,Zhu C L,Meng X,et al. Design and Fabrication of Ag-CuO Nanoparticles on Reduced Grapheme Oxide for Nonenzymatic Detection of Glucose[J]. Sens Actuators B,2018,265:435-442.
[18]	Li Y C,Zhong Y M,Zhang Y Y,et al. Carbon Quantum Dots/octahedral Cu2O Nanocomposites for Non-enzymatic Glucose and Hydrogen Peroxide Amperometric Sensor[J]. Sens Actuators B,2015,206:735-743.
[19]	Khan R,Ahmad R,Rai P,et al. Glucose-Assisted Synthesis of Cu2O Shuriken-Like Nanostructures and Their Application as Nonenzymatic Glucose Biosensors[J]. Sens Actuators B,2014,203:471-476.
[20]	Hou C T,Xu Q,Yin L N,et al. Metal-organic Framework Templated Synthesis of Co3O4 Nanoparticles for Direct Glucose and H2O2 Detection[J]. Analyst,2012,137(24):5803-5808.
[21]	Liu M M,Liu R,Chen W.Graphene wrapped Cu2O Nanocubes:Non-enzymatic Electrochemical Sensors for the Detection of Glucose and Hydrogen Peroxide with Enhanced Stability[J]. Biosens Bioelectron,2013,45:206-212.
[22]	Kung C W,Cheng Y H,Ho K C.Single Layer of Nickel Hydroxide Nanoparticles Covered on a Porous Ni Foam and Its Application for Highly Sensitive Non-enzymatic Glucose Sensor[J]. Sens Actuators B,2014,204:159-166.
[23]	Wang L,Xie Y Z,Wei C T,et al. Hierarchical NiO Superstructures/Foam Ni Electrode Derived from Ni Metal-Organic Framework Flakes on Foam Ni for Glucose Sensing[J]. Electrochim Acta,2015,174:846-852.
[24]	Jafarian M,Forouzandeh F,Danaee I,et al. Electrocatalytic Oxidation of Glucose on Ni and NiCu Alloy Modified Glassy Carbon Electrode[J]. J Solid State Electrochem,2009,13(8): 1171-1179.
[25]	HAO Miaoqing.Performance and Mechanism of the Direct Biomass Alkaline Fuel Cell[D]. Tianjin:Tianjin University,2013(in Chinese). 郝苗青. 直接生物质碱性燃料电池性能及机理研究[D]. 天津:天津大学,2013.
[26]	Dong C J,Tao Y,Chang Q,et al. Direct Growth of MnCO3 on Ni Foil for a Highly Sensitive Nonenzymatic Glucose Sensor[J]. J Alloys Compd,2018,762(25):216-221.
[27]	Zhang H Y,Liu S.Nanoparticles-Assembled NiO Nanosheets Templated by Graphene Oxide Film for Highly Sensitive Non-enzymatic Glucose Sensing[J]. Sens Actuators B,2017,238:788-794.
[28]	Fang B,Gu A X,Wang G F,et al. Silver Oxide Nanowalls Grown on Cu Substrate as an Enzymeless Glucose Sensor[J]. ACS Appl Mater Interfaces,2009,1(12):2829-2834.
[29]	Wang M,Ma Z Z,Li J P,et al. Well-dispersed Palladium Nanoparticles on Nickel-Phosphorus Nanosheets as Efficient Three-Dimensional Platform for Superior Catalytic Glucose Electro-oxidation and Non-enzymatic Sensing[J]. J Colloid Interface Sci,2018,511(4):355-364.