A highly sensitive non-enzymatic glucose sensor based on PtxCo1−x/C nanostructured composites

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Abstract

Platinum–cobalt (PtxCo1−x, x = 0.70, 0.55) alloy nanoparticles have been successfully fabricated by the chemical reduction method, using carbon (Vulcan XC-72) as support. The physical properties of the materials were characterized by X-ray diffraction, and transmission electron microscopy, respectively. The electrochemical performance of the PtxCo1−x/C catalysts was evaluated by cyclic voltammetry, electrochemical impedance spectroscopy and chronoamperometry. Electrochemical measurements indicated that the oxidation current of glucose is linear to its concentration from 0.10 to 14.20 mM with high sensitivity of 73.60 μA mM−1 cm−2. In addition, the interference from the oxidation of fructose, uric acid, acetamidophenol and ascorbic acid could be effectively avoided. Meanwhile, the non-enzymatic glucose sensors exhibited excellent selectivity, stability and repeatability. Thus, this novel non-enzyme sensor has potential application in glucose detection.

Introduction

Glucose is the main feature of the life process compounds, analysis and detection of it plays a very important role to human's healthy, especially for the diagnosis and management of diabetes mellitus [1], [2]. There are about 347 million people suffering from this disease worldwide according to the WHO in 2012. Hence, the development of simple, fast and efficient method for glucose detection becomes particularly significant.

The historical advances in the development of enzyme-based electrochemical glucose sensors commenced with Updike and Hicks reporting the first enzyme-based amperometric glucose sensor in 1967 [3]. Since then, enzyme-based glucose biosensors have been developing rapidly. However, enzyme-modified electrodes have some disadvantages, such as instability, the high cost of enzymes, complicated immobilization procedures, and critical operating conditions, so these sensors were not appropriate for applications [4].

To resolve these issues, the electrochemical glucose biosensors, especially non-enzymatic amperometric biosensors, with direct electrocatalytic oxidation of glucose at a non-enzymatic electrode have attracted much attention owing to their simplicity, high sensitivity, low cost, and compatibility toward miniaturization that would avoid the drawbacks of enzymatic sensors [5].

Metal nanoparticles (MNPs) have caused highly attention of researchers in modern chemistry and materials applications. Many non-enzymatic glucose sensors based on MNPs have been explored, especially Pt-based amperometric sensors [6], [7], [8], [9]. However, these kinds of glucose sensors present high cost, low sensitivity and selectivity caused by surface poisoning from the adsorbed intermediates [10], [11]. Therefore, the search for non-enzymatic glucose sensors more active and cheaper than Pt is very necessary. With these purposes, several Pt-based binary systems, such as Pt–Fe [12], [13], [14], [15], Pt–Ru [16], and Pt–Cu [17], with different Pt:M (M = a metal) atomic compositions have been investigated and have showed enhanced electrocatalytic activity toward the oxidation of glucose compared to Pt alone. Moreover, the presence of a second element could contribute to decreasing the costs associated with Pt.

In this work, the PtxCo1−x nanocomposites were fabricated by chemical reduction and used to modify a glassy carbon electrode surface. The results showed that the prepared PtxCo1−x/C NPs exhibited high electrocatalytic activity toward the oxidation of glucose and excellent stability for glucose determination. Therefore, the resulting nanocomposites could have potential utility for non-enzymatic glucose sensors.

Section snippets

Chemicals and reagents

Chloroplatinic acid (H2PtCl6·6H2O) and Cobalt chloride hexahydrate (CoCl2·6H2O) were purchased from Aldrich. Glucose was obtained from Guangcheng Chemical Reagent Co Ltd of Tianjin (Tianjin, China). Ascorbic acid (AA) was supplied by the Hubei University Chemical Factory (Hubei, China). Fructose, uric acid (UA), and acetamidophenol (AAP) were purchased from Aladdin. A 0.1 M phosphate buffer solution (PBS, 0.1 mol L−1, pH 7.0) was prepared using Na2HPO4 and KH2PO4. All aqueous solutions were

Characterization of the PtxCo1−x or Pt/C

Fig. 1A shows the X-ray diffraction patterns of PtxCo1−x alloys and Pt catalyst deposited on Vulcan XC-72 carbon. The diffraction peaks at 40° and 47° were indexed to Pt(1 1 1) and (2 0 0), respectively. All diffraction lines can be indexed to the face-centered cubic (fcc) phase of platinum (PC-PDF card No. 01-1194). Apart from the two strong diffraction peaks of Pt or PtxCo1−x phase, another broad diffraction peak at about 24° represents amorphous carbon. We noticed that the major diffraction

Conclusions

The bimetallic Pt0.55Co0.45/C and Pt0.7Co0.3/C nanocatalysts were prepared on the composite surface of carbon by using chemical reduction method. The obtained PtxCo1−x nanoparticles were well dispersed and exhibited the features of alloy. Electrochemical observation showed that the Pt0.7Co0.3/C modified electrode had large active surface areas and high electrocatalytic activity for the oxidation of glucose in PBS (pH 7.0) solutions. When it was used as a glucose sensor, the linear range,

Acknowledgement

We acknowledge financial support from the National Natural Science Foundation of China entitled “The synthesis of Pt-M/C nanoparticles and construction of non-enzymatic electrochemical biosensor” (Grant No. 21205030), and by the Education Department of the Hubei Province entitled “The development of non-enzymatic electrochemical biosensor based on Pt-M/C nanoparticles” (Q20120102), and from the Natural Science Fund for Creative Research Groups of Hubei Province of China through a project

Qu Sheng She is currently working toward the M.S. degree in College of Chemistry & Chemical Engineering, Hubei University. Her research interests include synthesis of nanomaterials for non-enzymatic glucose sensors.

References (35)

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Qu Sheng She is currently working toward the M.S. degree in College of Chemistry & Chemical Engineering, Hubei University. Her research interests include synthesis of nanomaterials for non-enzymatic glucose sensors.

He Mei He is currently working toward the M.S. degree in College of Chemistry & Chemical Engineering, Hubei University. His research interests include synthesis of nanomaterials for nanobiosensors and fuel cell.

Huimin Wu is an Associate Professor of Physical Chemistry at Hubei University. She holds a Ph.D. degree in Physical Chemistry from University of Wollongong, Australia. She received her M.S. degree in Physical Chemistry from Wuhan University. Her active areas of research include sensors, fuel cell, hydrogen storage, and nanomaterials.

Xiuhua Zhang is a Professor of Analytical Chemistry at Hubei University. His active areas of research include electrochemical sensor, bioelectrochemistry, electroanalytical chemistry, environmental analytical chemistry, and nanomaterials.

Shengfu Wang is a Professor of Analytical Chemistry at Hubei University. His active areas of research include electrochemical sensor, bioelectrochemistry, electroanalytical chemistry, environmental analytical chemistry, and nanomaterials.

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