Synthesis, characterization, and electrochemiluminescence of luminol-reduced gold nanoparticles and their application in a hydrogen peroxide sensor.

It was found that chloroauric acid (HAuCl(4)) could be directly reduced by the luminescent reagent luminol in aqueous solution to form gold nanoparticles (AuNPs), the size of which depended on the amount of luminol. The morphology and surface state of as-prepared AuNPs were characterized by transmission electron microscopy, UV/visible spectroscopy, X-ray photoelectron spectroscopy, FTIR spectroscopy, and thermogravimetric analysis. All results indicated that residual luminol and its oxidation product 3-aminophthalate coexisted on the surface of AuNPs through the weak covalent interaction between gold and nitrogen atoms in their amino groups. Subsequently, a luminol-capped AuNP-modified electrode was fabricated by the immobilization of AuNPs on a gold electrode by virtue of cysteine molecules and then immersion in a luminol solution. The modified electrode was characterized by cyclic voltammetry, electrochemical impedance spectroscopy, and scanning electron microscopy. The as-prepared modified electrode exhibited an electrochemiluminescence (ECL) response in alkaline aqueous solution under a double-step potential. H2O2 was found to enhance the ECL. On this basis, an ECL sensor for the detection of H2O2 was developed. The method is simple, fast, and reagent free. It is applicable to the determination of H2O2 in the range of 3x10(-7)-1x10(-3) mol L(-1) with a detection limit of 1x10(-7) mol L(-1) (S/N=3).

[1]  A. J. McQuillan,et al.  An In Situ Infrared Spectroscopic Study of the Adsorption of Lysine to TiO2 from an Aqueous Solution , 1998 .

[2]  M. Sastry,et al.  Investigation into the Interaction between Surface-Bound Alkylamines and Gold Nanoparticles. , 2003, Langmuir : the ACS journal of surfaces and colloids.

[3]  T. Eriksen,et al.  Oxidation potential of luminol: is the autooxidation of singlet organic molecules an outer-sphere electron transfer? , 1990 .

[4]  G G Guilbault,et al.  Recent applications of electrogenerated chemiluminescence in chemical analysis. , 2001, Talanta.

[5]  C. Hogan,et al.  Electrochemiluminescent metallopolymer coatings: combined light and current detection in flow injection analysis. , 2000, Analytical chemistry.

[6]  Han Nim Choi,et al.  Electrogenerated chemiluminescence from tris(2,2'-bipyridyl)ruthenium(II) immobilized in titania-perfluorosulfonated ionomer composite films. , 2003, Analytical chemistry.

[7]  C. Wang,et al.  Clay‐Enhanced Electrochemiluminescence and Its Application in the Detection of Glucose , 1998 .

[8]  Zhi‐Feng Zhang,et al.  Potential-dependent electrochemiluminescence of luminol in alkaline solution at a gold electrode , 2004 .

[9]  L. Murphy,et al.  Biosensors and bioelectrochemistry. , 2006, Current opinion in chemical biology.

[10]  Sihai Chen,et al.  Reversible Transference of Au Nanoparticles across the Water and Toluene Interface: A Langmuir Type Adsorption Mechanism , 2001 .

[11]  M. Sastry,et al.  On the stability of carboxylic acid derivatized gold colloidal particles: the role of colloidal solution pH studied by optical absorption spectroscopy , 1997 .

[12]  J. Turkevich,et al.  Coagulation of Colloidal Gold , 2002 .

[13]  Anand Gole,et al.  Water-dispersible tryptophan-protected gold nanoparticles prepared by the spontaneous reduction of aqueous chloroaurate ions by the amino acid. , 2004, Journal of colloid and interface science.

[14]  Sihai Chen,et al.  Synthesis and Characterization of Carboxylate-Modified Gold Nanoparticle Powders Dispersible in Water , 1999 .

[15]  G. Frens.  Controlled Nucleation for the Regulation of the Particle Size in Monodisperse Gold Suspensions , 1973 .

[16]  Haisheng Tao,et al.  Electrochemical and Electrocatalytic Properties of Ferrocene Incorporated in L‐Cysteine Self‐Assembled Monolayers on a Gold Electrode , 2006 .

[17]  G. Southam,et al.  Morphology of gold nanoparticles synthesized by filamentous cyanobacteria from gold(I)-thiosulfate and gold(III)--chloride complexes. , 2006, Langmuir : the ACS journal of surfaces and colloids.

[18]  E. Wang,et al.  Capillary electrophoresis coupling with electrochemiluminescence detection: a review , 2005 .

[19]  H. Cui,et al.  Determination of noradrenaline and dopamine in pharmaceutical injection samples by inhibition flow injection electrochemiluminescence of ruthenium complexes. , 2003, Talanta.

[20]  H. Cui,et al.  Electrochemiluminescence of luminol in alkaline solution at a paraffin-impregnated graphite electrode. , 2003, Analytical chemistry.

[21]  Jing-Juan Xu,et al.  Reagentless chemiluminescence biosensor for determination of hydrogen peroxide based on the immobilization of horseradish peroxidase on biocompatible chitosan membrane , 2002 .

[22]  Andrew W. Knight,et al.  A review of recent trends in analytical applications of electrogenerated chemiluminescence , 1999 .

[23]  Shaojun Dong,et al.  A novel alcohol dehydrogenase biosensor based on solid-state electrogenerated chemiluminescence by assembling dehydrogenase to Ru(bpy)(3)2+-Au nanoparticles aggregates. , 2007, Biosensors & bioelectronics.

[24]  S. Dong,et al.  Synthesis of gold nanoplates by aspartate reduction of gold chloride. , 2004, Chemical communications.

[25]  Stephan Link,et al.  Size and temperature dependence of the plasmon absorption of colloidal gold nanoparticles , 1999 .

[26]  John F. Watts,et al.  Preparation and characterisation of gold nanoparticle assemblies on silanised glass plates , 2003 .

[27]  S. Dong,et al.  Electrochemistry and electrogenerated chemiluminescence of SiO2 nanoparticles/tris(2,2 '-bipyridyl)ruthenium(II) multilayer films on indium tin oxide electrodes , 2004 .

[28]  G. Ramanath,et al.  Diffusion barrier properties of carboxyl- and amine-terminated molecular nanolayers , 2004 .

[29]  Imdadullah,et al.  Chemiluminescence from the reaction of chloroauric acid with luminol in reverse micelles , 1991 .

[30]  Michal Lahav,et al.  Investigations into the Electrostatically Induced Aggregation of Au Nanoparticles , 2000 .

[31]  James R. Heath,et al.  Synthesis and Characterization of Hydrophobic, Organically-Soluble Gold Nanocrystals Functionalized with Primary Amines , 1996 .

[32]  Zhi‐Feng Zhang,et al.  Multichannel electrochemiluminescence of luminol in neutral and alkaline aqueous solutions on a gold nanoparticle self-assembled electrode. , 2004, Analytical chemistry.

[33]  Yan Du,et al.  Method for effective immobilization of Ru(bpy)(3)2+ on an electrode surface for solid-state electrochemiluminescene detection. , 2005, Analytical chemistry.

[34]  P. Perriat,et al.  Synthesis, characterization of dihydrolipoic acid capped gold nanoparticles, and functionalization by the electroluminescent luminol. , 2005, Langmuir : the ACS journal of surfaces and colloids.

[35]  Nicholas J. Turro,et al.  Photolithographic technique for direct photochemical modification and chemical micropatterning of surfaces , 2004 .

[36]  Baoxin Li,et al.  Chemiluminescent flow-through sensor for hydrogen peroxide based on sol–gel immobilized hemoglobin as catalyst , 2001 .

[37]  Electrode surface modification by a spirobifluorene derivative. An XPS and electrochemical investigation. , 2005, The journal of physical chemistry. B.

[38]  Aimin Yu,et al.  Direct electron transfer and characterization of hemoglobin immobilized on a Au colloid-cysteamine-modified gold electrode , 2001 .

[39]  O. Nozaki,et al.  Reactivation of inactivated horseradish peroxidase with ethyleneurea and allantoin for determination of hydrogen peroxide by micro-flow injection horseradish peroxidase-catalyzed chemiluminescence , 2003 .

[40]  M. Srinivasan,et al.  Covalent molecular assembly in supercritical carbon dioxide: a comparative study between amine- and anhydride-derivatized surfaces. , 2006, Langmuir : the ACS journal of surfaces and colloids.

[41]  Priyabrata Mukherjee,et al.  Phase transfer of aqueous colloidal gold particles into organic solutions containing fatty amine molecules , 2001 .

[42]  Vinayak P. Dravid,et al.  Novel one-step synthesis of amine-stabilized aqueous colloidal gold nanoparticles , 2004 .

[43]  F. Caruso,et al.  Phase transfer of surface-modified gold nanoparticles by hydrophobization with alkylamines , 2003 .

[44]  Shaojun Dong,et al.  Electrogenerated chemiluminescence from R(bpy)3(2+) ion-exchanged in carbon nanotube/perfluorosulfonated ionomer composite films. , 2004, Analytical chemistry.

[45]  I. Willner,et al.  Layered Polyelectrolyte Films on Au Electrodes: Characterization of Electron-Transfer Features at the Charged Polymer Interface and Application for Selective Redox Reactions , 2001 .

[46]  Joseph Wang.  Nanomaterial-based amplified transduction of biomolecular interactions. , 2005, Small.

[47]  G. Blanchard,et al.  Formation of gold nanoparticles using amine reducing agents. , 2006, Langmuir : the ACS journal of surfaces and colloids.

[48]  G. Merényi,et al.  Chemiluminescence mechanism of cyclic hydrazides such as luminol in aqueous solutions , 1983 .

[49]  Xingwang Zheng,et al.  A novel electrogenerated chemiluminescence sensor for pyrogallol with core-shell luminol-doped silica nanoparticles modified electrode by the self-assembled technique. , 2006, Analytica chimica acta.