AgNPs/聚萘二胺/碳纳米管复合电极对亚硝酸盐的电化学检测
Electrochemical detection of nitrite based on silver nanoparticles/poly (naphthalenediamine)/carbon nanotubes composites electrode
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摘要: 本文采用简单、环保的电化学沉积法制备银纳米粒子/聚萘二胺/碳纳米管修饰玻碳电极（AgNPs/Poly（1，5-DAN）/CNTs/GCE），并将其应用于亚硝酸盐的定量检测.通过扫描电子显微镜（SEM）、能量散射光谱（EDX）和电化学技术对AgNPs/Poly（1，5-DAN）CNTs/GCE的形貌和性能进行表征，研究该修饰电极快速检测NO2-离子的电化学行为和电催化机理.结果表明，由于银纳米粒子、聚萘二胺和碳纳米管复合物的协同作用，AgNPs/Poly（1，5-DAN）CNTs/GCE复合电极的电活性面积和催化性能明显提高.该修饰电极对NO2-的检测具有优异的电化学行为，催化机理是2个电子参与的不可逆反应.采用安培法检测低浓度NO2-，NO2-氧化电流随其浓度的增加而增加，且在1.5×10-7-6.75×10-5 mol·L-1（I（μA）=0.0667 C+0.1049，R2=0.9918）范围内呈现良好的线性关系，检出限低至5×10-8 mol·L-1（S/N=3）.该AgNPs/Poly（1，5-DAN）CNTs/GCE还具有良好的选择性、稳定性和再现性，成功应用于实际样品中NO2-的定量测定，加标回收率为96.7%-106.7%，结果令人满意.Abstract: In this paper, the silver nanoparticles/poly(naphthalenediamine)/carbon nanotubes modified glassy carbon electrode (AgNPs/Poly(1,5-DAN)/CNTs/GCE) was prepared by a simple and environmental-friendly electrodeposition method, which was applied to quantitatively detect the nitrite (NO2-) salts. The morphology and properties of AgNPs/Poly(1,5-DAN)/CNTs/GCE were characterized by scan electron microscope (SEM), energy dispersive X-ray spectrum (EDX) and electrochemical techniques. The electrochemical behavior and electrocatalytical mechanism of nitrite detection were also examined. The results displayed that the electroactive area and catalytical properties of AgNPs/Poly(1,5-DAN)/CNTs/GCE were significantly improved, mainly due to the synergistic effects of AgNPs, poly(1,5-DAN) and CNTs. The proposed electrode had excellent electrochemical behaviors for the determination of NO2-, and the catalytical mechanism was involved two electrons in irreversible reaction. The low concentration of NO2- was detected by amperometry, and the oxidation peak currents of nitrite were increased with the increasement of its concentration. The good linearity of peak currents versus NO2- concentration was obtained in the range of 1.5×10-7-6.75×10-5 mol ·L-1 (I (μA)=0.0667 C+ 0.1049, R2=0.9918), and the limit of detection (LOD) was as low as 5×10-8 mol ·L-1(S/N=3). The AgNPs/Poly(1,5-DAN)/CNTs/GCE had good selectivity, long-term stability and reproductivity, which was successfully applied to detect nitrite in real water samples. The recovery rates of standard addition were ranging from 96.7% to 106.7% with satisfactory results.
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Key words:
- silver nanoparticles /
- poly(naphthalenediamine) /
- nitrite /
- electrocatalytical oxidation
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[1] GAYEN P, SPATARO J, AVASARALA S, et al. Electrocatalytic reduction of nitrate using magneli phase TiO2 reactive electrochemical membranes doped with Pd-based catalysts[J]. Environmental Science & Technology, 2018, 52(16):9370-9379. [2] 李思倩,路立,王芬,等. 低温反硝化过程中pH对亚硝酸盐积累的影响[J].环境化学,2016, 35(8):1657-1622. LI S Q, LU L, WANG F, et al. Effect of pH on nitrite accumulation during denitrification at low temperature[J]. Environmental Chemistry, 2016, 35(8):1657-1622(in Chinese).
[3] LI B L, LI Y S, GAO X F. Fluorescence quenching capillary analysis for determining trace-level nitrite in food based on the citric acid/ethylenediamine nanodots/nitrite reaction[J]. Food Chemistry, 2019, 274:162-169. [4] 徐霞,应兴华,陈能,等.离子色谱法同时测定蔬菜中的亚硝酸盐与硝酸盐[J].环境化学,2005, 24(6):733-734. XU X, YING X H, CHEN N, et al. Simultaneous determination of nitrite and nitrate in vegetables by ion chromatography[J]. Environmental Chemistry, 2005, 24(6):733-734(in Chinese).
[5] FABIANA D B, LUCIANO V, ROSEANE F, et al. Development and validation of a sub-minute capillary zone electrophoresis method for determination of nitrate and nitrite in baby foods[J]. Talanta, 2014, 122:23-29. [6] YANG J, YANG L T, YE H L, et al. Highly dispersed AuPd alloy nanoparticles immobilized on UiO-66-NH2 metal-organic framework for the detection of nitrite[J]. Electrochimica Acta, 2016, 219:647-654. [7] KURALAY F, DUMANGÖZ M, TUN. Polymer/carbon nanotubes coated graphite surfaces for highly sensitive nitrite detection[J]. Talanta, 2015, 144:1133-1138. [8] RAJALAKSHMI K, JOHN S A. Highly sensitive determination of nitrite using FMWCNTs-conducting polymer composite modified electrode[J]. Sensors and Actuators B:Chemical, 2015, 215:119-124. [9] LI G X, HUANG M R, DUAN W, Novel multifunctional polymers from aromatic diamines by oxidative polymerizations[J]. Chemical Reviews, 2002, 102(9):2925-3030. [10] RIOJAS A A C, WONG A, PLANES G A, et al. Development of a new electrochemical sensor based on silver sulfide nanoparticles and hierarchical porous carbon modified carbon paste electrode for determination of cyanide in river water samples[J]. Sensors and Actuators B:Chemical, 2019, 287:544-550. [11] THIRUMALRAJ B, PALANISAMY S, CHEN S M, et al. Amperometric detection of nitrite in water samples by use of electrodes consisting of palladium-nanoparticle-functionalized multi-walled carbon nanotubes[J]. Journal of Colloid and Interface Science, 2016, 478:413-420. [12] BARD A J, FAULKNER L R, Electrochemical methods-fundamentals and applications[M]. New York:John Wiley and Sons, 2000. [13] CASELLA I G, CONTURSI M. Highly dispersed rhodium particles on multi walled carbon nanotubes for the electrochemical reduction of nitrate and nitrite ions in acid medium[J]. Electrochimica Acta, 2014, 138:447-453. [14] AFKHAMI A, SOLTANI-FELEHGRRI F, MADRAKIAN T, et al. Surface decoration of multi-walled carbon nanotubes modified carbon paste electrode with gold nanoparticles for electro-oxidation and sensitive determination of nitrite[J]. Biosensors and Bioelectronics, 2014, 51:379-385. [15] RHAZI M E, MAJID S. Electrochemical sensors based on polydiaminonaphthalene and polyphenylenediamine for monitoring metal pollutants[J]. Trends in Environmental Analytical Method, 2014, 2:33-42. [16] BADEA M, AMINE A, PALLESCHI G, et al. New electrochemical sensors for detection of nitrites and nitrates[J]. Journal of Electroanalytical Chemistry, 2001, 509:66-72. [17] GLIGOR D, WALCARIUS A. Glassy carbon electrode modified with a film of poly(Toluidine Blue O) and carbon nanotubes for nitrite detection[J]. Journal of Solid State Electrochemistry, 2017, 18:1519-1528. [18] LIU Y, ZHOU J, GONG J, et al. The investigation of electrochemical properties for Fe3O4@Pt nanocomposites and an enhancement sensing for nitrite[J]. Electrochimica Acta, 2013, 111:876-887. [19] KUNG C W, CHANG T H, CHOU L Y, et al. Porphyrin-based metal-organic framework thin films for electrochemical nitrite detection[J]. Electrochemistry Communications, 2015, 58:51-56. [20] ZHANG D, FANG Y X, MIAO Z Y, et al. Direct electro-deposition of reduced graphene oxide and dendriticcopper nanoclusters on glassy carbon electrode for electrochemical detection of nitrite[J]. Electrochimica Acta, 2013, 107:656-663. [21] RAMACHANDRAN K, KALPANA D, SATHISHKUMAR Y, et al. A facile green synthesis of silver nanoparticles using Piper betle biomass and its catalytic activity toward sensitive and selective nitrite detection[J]. Journal of Industrial and Engineering Chemistry, 2016, 35:29-35. [22] BAI W S, SHENG Q L, ZHENG J B. Hydrophobic interface controlled electrochemical sensing of nitrite based on one step synthesis of polyhedral oligomeric silsesquioxane/reduced graphene oxide nanocomposite[J]. Talanta, 2016, 150:302-309. [23] YADAV M K, GANESAN V, SONKAR P K, et al. Electrochemical investigation of gold nanoparticles incorporated zinc based metal-organic framework for selective recognition of nitrite and nitrobenzene[J]. Electrochimica Acta, 2016, 200:276-282. [24] MEHMETI E, STANKOVIĆ D M, HAJRIZI A, et al. The use of graphene nanoribbons as efficient electrochemical sensing material for nitrite determination[J]. Talanta, 2016, 159:34-39. [25] ZHANG S, LI B Q, SHENG Q L, et al. Electrochemical sensor for sensitive determination of nitrite based on the CuS-MWCNT nanocomposites[J]. Journal of Electroanalytical Chemistry, 2016, 769:118-123. [26] ZOU C E, YANG B B, BIN D, et al. Electrochemical synthesis of gold nanoparticles decorated flower-like graphene for high sensitivity detection of nitrite[J]. Journal of Colloid and Interface Science, 2017, 488:135-141. [27] SILVA S M D, MAZO L H. Differential pulse voltammetric determination of nitrite with gold ultramicroelectrode[J]. Electroanalysis, 1998, 10:1200-1203. [28] 叶小爱,章家立,关婷婷,等.二氧化锰/石墨烯/N-取代羧基聚苯胺复合修饰电极对亚硝酸根的电化学催化研究[J]. 分析测试学报, 2018, 37(1):39-44. YE X A, ZHANG J L, GUAN T T, et al. Electrocatalytic study of nitrite based on MnO2/rGO/NPAN composite film modified electrode[J]. Journal of Instrumental Analysis, 2018, 37(1):39-44(in Chinese).
[29] 任聚杰,于聪聪,崔敏, 等.基于氯化血红素复合材料的过氧亚硝酸阴离子电化学传感器的构建[J]. 分析化学,2017, 45(1):104-110. REN J J, YU C C, CUI M, et al. Construction of hemin composite based electrochemical sensor for detection of peroxynitrite[J]. Chinese Journal of Analytical Chemistry, 2017, 45(1):104-110(in Chinese).
[30] 张娜,张克营,朱萍萍,等. 聚天青Ⅰ/石墨烯修饰电极的电化学行为及对亚硝酸根的检测[J]. 分析试验室,2015, 34(7):816-818. ZHANG N, ZHANG K Y, ZHU P P, et al. The electrochemical behaviors of poly (azure Ⅰ)/graphene modified electrode and its application for nitrite detection[J]. Chinese Journal of Analytical Laboratory, 2015, 34(7):816-818(in Chinese).
[31] HUI N, CHAI F L, LIN P P, et al. Electrodeposited conducting polyaniline nanowire arrays aligned on carbon nanotubes network for high performance supercapacitors and sensors[J]. Electrochimica Acta, 2016, 199:234-241. [32] RAO D J, SHENG Q L, ZHENG J B. Self-assembly preparation of gold nanoparticle decorated 1-pyrenemethylamine functionalized graphene oxide-carbon nanotube composites for highly sensitive detection of nitrite[J]. Analytical Methods, 2016, 8:4926-4933. [33] ZHANG S, LIU X Y, HUANG N, et al. Sensitive detection of hydrogen peroxide and nitrite based on silver/carbon nanocomposite synthesized by carbon dots as reductant via one step method[J]. Electrochemica Acta, 2016, 211:36-43. -
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