Vous êtes sur la page 1sur 7

Sensors and Actuators B 177 (2013) 555561

Contents lists available at SciVerse ScienceDirect


Sensors and Actuators B: Chemical
j our nal homepage: www. el sevi er . com/ l ocat e/ snb
Self-made non-enzymatic silver electrode from recordable CDs for fast detection
of glucose in blood
Yuxing Chen
a
, Lin Liu
a
, Meirong Wang
a
, Chengyin Wang
a,
, Xiaoya Hu
a
, Guoxiu Wang
b
a
College of Chemistry and Chemical Engineering, Jiangsu Key Laboratory of Environmental Engineering and Monitoring, Yangzhou University, 180 Si-Wang-Ting Road,
Yangzhou 225002, China
b
Department of Chemistry and Forensic Science, University of Technology, Sydney, City Campus, Broadway, Sydney, NSW2007, Australia
a r t i c l e i n f o
Article history:
Received 11 August 2012
Received in revised form
18 November 2012
Accepted 19 November 2012
Available online 29 November 2012
Keywords:
Recordable CDs
Non-enzymatic sensor
Chronoamperometry
Glucose
Blood
a b s t r a c t
An electrochemical sensor based on a self-made electrode from recordable CDs was developed for the
non-enzymatic detection of glucose by chronoamperometry. We discussed the amperometric current
response of glucose with the change of potential, pH and electrode area, and determined the optimum
detection conditions. The current response measurements were performed in a phosphate buffered solu-
tion (pH 6.5) with a potential of 0.50V, and presented a linearity over the range of 0.513 mmol/L
(r = 0.996). The experimental results of the designed sensor demonstrate that this method has merits
such as simple operation, low cost and rapid responses. The results of detecting glucose in blood samples
were satisfactory.
2012 Elsevier B.V. All rights reserved.
1. Introduction
Glucose detection is extremely important in the diagnoses and
treatment of diabetes patients. Diabetes is a disease resulting from
hyperglycemia and insulin deciency, and leads to complications
such as renal, retinal, cardiac and neural pathema [1]. The compli-
cations can be reduced through strictly controlled personal blood
glucose [2]. Increasingly, more diabetic patients have to measure
their blood glucose levels regularly each day. Therefore, a fast and
reliable methodof monitoring the bloodglucose level is needed[3].
Recently, many techniques have been undertaken for the determi-
nation of blood glucose. For example, Ayupe de Oliveira et al. [4]
developed a spectrophotometric method for the determination of
blood glucose, and used an on-line tubular reactor with glucose
oxidase immobilized on resin. Der and Dattelbaum[5] constructed
a uorescent glucose/galactose binding protein (GGBP) biosensor,
used to set up double-cysteine mutations that allowed the selec-
tive covalent attachment of thiol-reactive dyes. Pleitez et al. [6]
established a newinfrared spectroscopic analysis approach to non-
invasive glucose measurement. However, there has been more
focus on electrochemical methods of glucose detection in recent
years because of numerous advantages, such as simple and rapid
operation, high sensitivity and lowdetection limits.

Corresponding author. Tel.: +86 514 87888454; fax: +86 514 87975244.
E-mail addresses: wangcy@yzu.edu.cn, yzswcy@yzcn.net (C. Wang).
Electrochemical glucose sensors began with glucose enzyme
electrodes, which were quickly developed. The sensors are based
on the enzyme glucose oxidase (GOx); and the GOx works
through redox reactions with glucose. During the interaction,
hydrogen peroxide is generated, which is formed as a redox
mediator, and produces the redox signal. Many glucose biosen-
sors are dependent on the electrochemical oxidation of hydrogen
peroxide, and can be detected through oxidation at high poten-
tials. Zhou et al. [7] proposed a new glucose sensor, containing
m-phenylenediamine and glucose oxidase (GOx), by the elec-
tropolymerizationof m-phenylenediamine inthe phosphate buffer
solution. Liu [8] fabricated an enzyme electrode, based on a self-
assembled Prussian Blue (PB) and glucose oxidase (GOD) modied
electrode. However, there may be interferences from common
interfering species, such as ascorbic acid (AA) and uric acid (UA),
which cause serious difculties for the determination of glucose
[9]. Inaddition, the catalytic activity of GOx is impactedby environ-
mental conditions suchas temperature, humidity, pHvalue, organic
reagents, and oxygen restriction, which would affect the sensitivity
and specicity [10]. Furthermore, GOx is relatively expensive. The
disadvantages limit the widespread use of the enzyme-modied
electrodes. Therefore, the development of non-enzymatic glucose
sensors is necessary.
Non-enzymatic amperometric sensors for direct determination
of glucose has attracted great interest from researchers in recent
years, and many enzymeless glucose sensors have been developed
withnoblemetal nanoparticles (Pt, AuandPd) [11,12], metal oxides
0925-4005/$ see front matter 2012 Elsevier B.V. All rights reserved.
http://dx.doi.org/10.1016/j.snb.2012.11.061
556 Y. Chen et al. / Sensors and Actuators B 177 (2013) 555561
(CuO, Co
3
O
4
, NiO, etc.) [1315], metal alloys (PtPb, PtRu, PtAu,
NiPd, etc.) [1618], and nano-composites [19,20]. These non-
enzymatic glucose sensors have been reported to have remarkable
qualities, such as lower cost, faster response time, stability and the
independenceof oxygen. But there is noreport onglucose detection
directly with Ag-NPs modied electrodes.
Compact discs (CDs) are a formof optical data storage contain-
ing a nanometric metal layer such as gold, silver or aluminum. The
metal layers from CDs as electrodes can be called CDtrodes. The
CDtrodes have many advantages, such as low-cost, easy handling,
and disposable surface. Because of the many benets, CDtrodes
have been applied to electrochemical and biochemical analysis.
A variety of literature is reported to show the applications of
CDtrodes. Ba nuls et al. [21] demonstrated several approaches to
the covalent modication of CDs and applied them to DNA probe
immobilization, hybridization, and SNP (single nucleotide poly-
morphisms) discrimination assays on polycarbonate disc surfaces.
Morais et al. [22] performed high-density competitive indirect
microimmunoassays based on a low-reectivity compact disc as
analytical platform. Challener et al. [23] designed a surface plas-
mon resonance (SPR) gas sensor using a rotating optical disc to
detect ammonia, whichcaneasilybe extendedtomultiple channels
and is inexpensive. Tamarit-Lpez et al. [24] presented an analyt-
ical potential for polystyrene (PS) spin-coated modied compact
disc (CD) surfaces as platforms for the development of microar-
ray immunoassays. Alexandre et al. [25] proposed a compact disc
as a support for constructing DNA microarrays suited to genomic
analysis.
In this paper, we developed a non-enzymatic glucose sensor for
CDs by coating a reective metal layer withsilver, whichperformed
with the same advantages of metal nanoparticles modied elec-
trodes. The extreme signicance of this work is the recycling of
recordable CDs, as well as the simple and easy preparation of the
CDtrodes. What is important is that the low cost of CDtrodes and
the electrode area can be easily modied according to the needs of
the experiments. The response of the proposedelectrode to glucose
concentrations was linear over the range of 0.513mmol/L. The
CDtrode can be used to determine the blood glucose directly, and
the interference of ascorbic acid (AA) and uric acid (UA) are effec-
tively avoided. Here we provide a possible methodfor the detection
of glucose in human blood.
2. Experimental
2.1. Reagent
Concentrated nitric acid, uric acid, and sodium dihydrogen
phosphates were purchased from Sinopharm Chemical Reagent
Co. Ltd. (Shanghai, China). Ascorbic acid and uric acid were pur-
chased fromGuangzhou Chemical Reagent Company (Guangzhou,
China). The phosphate buffer solutions (PBS) (0.1mol/L) were pre-
pared fromNaH
2
PO
4
and Na
2
HPO
4
. All the other chemicals were of
analytical reagent grade, and used without further purication. All
water used for preparing the solutions inthis work was re-distilled.
2.2. Apparatus
Electrochemical experiments were performed with a CHI 1232
electrochemical workstation (Chenhua Instruments Company,
Shanghai, China) with a conventional three-electrode system. The
self-madeCDsilver electrodes, anAg/AgCl anda platinumelectrode
were used as the working electrode, reference and the auxil-
iary electrode, respectively. Scanning Electron Microscope (SEM)
measurements were conducted on an S-4800|| FESEM (Hitachi
High-Technologies Corporation, Japan) at anaccelerating voltage of
20kV. 85-1 magnetic stirrers (KeEr Instruments Company, Nanjing,
China) and a Mettler-Toledo FE20 pHmeter (Shanghai, China) were
adopted. All experiments were carried out at room temperature
(25

C).
2.3. Composition of recordable compact disc and preparation of
the CD electrode
RecordableCDs usedinthis workwereobtainedfromRITEKCor-
poration (CD-R 52X, 5.25in.). This kind of CD contains four parts:
(a) a polycarbonate of high durability provides the mechanical sup-
port tothe unit andoffers protectionfor the discs [26,27]. (b) Onthe
above-mentioned layer, a thin layer of photosensitive organic dye
is deposited, whichcanbe constitutedwithazogroups, phthalocya-
nine, or metal-stabilizedcyanine [28]. (c) Over the secondlayer, the
recording progress was performed by use of a reective metal layer
of between 50 and 100nm. This layer usually is made of gold, silver,
or aluminum[29], but in recent years more CDs have silver or gold
instead of aluminum as the reective layer, with silver reectors
showing better performance. (d) This metal layer is covered again
with two polymeric protecting lms: one lmis a lacquer that pro-
tects the reective lmand the other accepts the ink fromprinters
[30].
The compact disc was divided into many parts, and each part
offered several electrodes. To obtain the thin reective layer
demanded, a pair of scissors was employed. The CDs were cut
into 1016 slices, like a pizza. To construct the CD electrodes,
it was necessary to remove the protective lm from its surface.
Some researchers reported the process to expose the reective
layer after a chemical attack to protecting lms [26,28]. In our
experiment, the thin metal lm with irregular shape was easily
peeled off with a knife and tweezers. Subsequently, the Ag lm
was cut into strips with widths of 0.5cm and lengths of 2.0cm
in order to be convenient on next cleaning step. The lm strips
were washed with absolute alcohol to remove organics. And
then, 3mm3mm Ag lm was tailored from the strip as the
working electrode according to our electrochemical cell designed
(Fig. 1(A)). We referred to a screen printed structure based on the
3-electrode electrochemical cell to propose our sensor, but the
regular working electrode was replaced by Ag lm from CD-R.
Details of its fabrication are provided as below: working, counter
and reference electrodes covered onto a PVC substrate. For counter
and reference electrode, the metallic layer was printed using the
platinum and Ag/AgCl inks. For working electrode, a sheet of Ag
lm (3mm3mm) was adhered to the working electrode site
Fig. 1. Images of the portable glucose sensor (A) and the portable glucose sensor
connected to the USB port (B). (a) the self-made silver CDs electrode, (b) a platinum
electrode, (c) Ag/AgCl electrode, (d) an insulating coat, (e) PVC substrate.
Y. Chen et al. / Sensors and Actuators B 177 (2013) 555561 557
with a kind of conducting glue. Then an insulator layer was placed
over the conducting paths (1mm width). The proposed sensor is
a portable glucose sensor, which is like a USB ash with a USB
port to connect to an electrochemical workstation, as shown in
Fig. 1(B). This device was applied directly to detect blood glucose.
This strategy will probably be commercialized in the future.
2.4. Electrochemical test
The electrochemical characterization of the CDtrode was evalu-
ated by using cyclic voltammetry (CV) in 0.1mol/L PBS. The current
response measurements were performed in a phosphate buffered
solution (pH 6.5, C=0.1mol/L) with a potential of 0.50V, and the
detection of glucose concentration in human blood was performed
under the same conditions.
3. Results and discussion
3.1. Characterization of the CD electrode
A representative SEM image of a CDtrode, as shown in Fig. 2,
clearly indicates nanoparticles uniformly attached to the electrode
surface, with an average diameter of about 20nm. The Energy Dis-
persiveX-rayspectroscopy(EDX) dateimageof theCDtrodeinFig. 3
shows that the substance in the lm was Ag nanoparticles. When
this lmwas used as an electrode material, the CDtrode became an
Ag nanoparticles electrode.
To characterize the electrochemical behavior of the self-made
CDtrode, a cyclic voltammogram(CV) of the CDtrode (Fig. 4(A)) in
0.1mol/L H
2
SO
4
solution was compared with one of a commercial
silver electrode (Fig. 4(B)). The two peaks, one anodic (situatednear
Fig. 2. SEMimage of CDtrode.
to 0.60V) and the other cathodic (at 0.30V), were observed. Both
CVs presented practically the same shape, which indicated that the
self-made CDtrode had the same properties as a commercial silver
electrode.
3.2. Voltammetric response to glucose
Voltammetric responses to different glucose levels were
recorded with scan rate of 50mV/s and potential range from0.7V
to 0V in Fig. 5. The experimental result indicated that the cur-
rent response increased with increasing glucose concentration.
Fig. 3. The EDX results of CDtrode.
-0.4 -0.2 0.0 0.2 0.4 0.6 0.8 1.0 1.2 1.4
-3
-2
-1
0
1
2
3
C
u
r
r
e
n
t

/

A
Potential / V
-0.4 -0.2 0.0 0.2 0.4 0.6 0.8 1.0 1.2 1.4
-2.5
-2.0
-1.5
-1.0
-0.5
0.0
0.5
1.0
1.5
2.0
C
u
r
r
e
n
t

/

m
A
Potential / V
a b
Fig. 4. The cyclic voltammograms of a CDtrode (A) and a commercial electrode (B) recorded in 0.1mol/L H
2
SO
4
by sweeping the potential between 0.4V and 1.3V at a scan
rate of 50mV/s.
558 Y. Chen et al. / Sensors and Actuators B 177 (2013) 555561
-0.8 -0.7 -0.6 -0.5 -0.4 -0.3 -0.2 -0.1 0.0 0.1
0
2
4
6
8
10
12
d
c
b
C
u
r
r
e
n
t

/

A
Potential / V
a
Fig. 5. The cyclic voltammograms of the CDtrode in 0.1mol/L PBS containing glu-
cose with scan rate of 50mV/s and potential range from0.7V to 0V. (a) Blank, (b)
0.1mmol/L glucose, (c) 0.5mmol/L glucose, and (d) 3mmol/L glucose.
The AgNPs electrode gives the high catalytic activity toward glu-
cose oxidation in a neutral phosphate buffer provides a tentative
electrode reaction for the oxidation of glucose at 0.5V. The
voltammetric response on glucose concentration in neutral and
alkalinemediummight beduetotheglucoseoxidationontheinux
of OH

[17]. In the presence of glucose, glucose molecules were


electro-absorbed on the surface of the CDtrode, forming a layer
of glucose intermediates. With the potential scanning to 0.5V,
the adsorbed glucose intermediates were oxidized on the electrode
surface, causing the increase of the current [18]. Referring to a liter-
ature [31] a tentative electrode reactionfor the oxidationof glucose
was showninScheme1. It has beenreasonedthat theweaklybound
hydrogen atomat the carbon C atomis the rst to be detached from
the glucose molecule at the electrode poised at lowpotentials.
3.3. Effect of the potential on the response current
Potential controllability is one of the key parameters in
chronoamperometry. Fig. 6 shows the potential effect of the oper-
ation on the amperometric response to detect 4.0mmol/L glucose.
On the CDtrode surface, glucose oxidation exhibited strong elec-
trocatalytic activity at a negative potential of 0.50V. According
to Guo et al. [18], this is probably because glucose molecules were
adsorbed onto the CDtrode surface and formed a layer of glucose
intermediates. The intermediates could be oxidized on the CDtrode
surface when the potential was 0.50V, resulting in the increase
of the current. The response current decreased when the potential
was further moved from0.50V. The glucose intermediates were
oxidized with difcultly at a more negative potential, and Ag-NPs
could be oxidized with the increase of potential. So the potential of
0.50V was chosen as the optimumpotential in our experiments.
Guo et al. proposed a PtPb nanostructures modied electrode to
detect glucose at a negative potential of 0.1V, the interference
of ascorbic acid and uric acid effectively was avoided at a negative
potential [18]. Huang and Zhu reported that the graphene and Au-
NPs modied electrode exhibited good amperometric response to
glucose at 0.2V, with good reproducibility [32].
O
R
C OH
H
Ag
Adsorption
O
R
C OH
X
+ H
+
+ e
-
Scheme 1. Electrochemical reaction on the CDtrode.
-0.8 -0.7 -0.6 -0.5 -0.4 -0.3 -0.2 -0.1 0.0 0.1
-2
0
2
4
6
8
10
12
14
C
u
r
r
e
n
t

/

A
Potential /V
Fig. 6. Effect of the potential on the CDtrode response. Steady-state currents were
measured in 0.1mol/L phosphate buffer (pH 7.0) containing glucose 4.0mmol/L.
3.4. Effect of the value of pH on the response current
Fig. 7 shows the effect of pH values on the response current
when pH values varied from 5.0 to 9.0 in the solution containing
4.0mmol/L glucose. With the increase of pH, the response currents
of the glucose onthe CDtrode were increased, andreachedthe max-
imumvalue at pH6.5. While in base solutions, OH

would enhance
Ag oxidation, and the CDtrodes were damaged. Therefore, the pH
value of 6.5 was chosen to detect glucose, which is much closer to
physical conditions in human blood.
3.5. Effect of the CDtrode area on the response current
It is known that the electrode area strongly affects the response
current. In order to get the stable current response, different elec-
trode areas were chosenfor the detectionof glucose. The increase of
electrode area could generate the increase of the current response,
but stabilityof the current became worse andnoise increased. Thus,
the area should be controlled within as small a space as possible.
We chose 3mm3mmof CDtrode area in our experiment.
5 6 7 8 9
-4
-2
0
2
4
6
8
10
12
14
16
C
u
r
r
e
n
t

/

A
pH
Fig. 7. Effect of the pH on the CDtrode response. Steady-state currents were mea-
sured at 0.50V in 0.1mol/L phosphate buffer containing glucose 4.0mmol/L.
Y. Chen et al. / Sensors and Actuators B 177 (2013) 555561 559
0 100 200 300 400 500 600
6
8
10
12
14
145 150 155 160
7.4
7.6
7.8
8.0
8.2
C
u
r
r
e
n
t
/

A
C
u
r
r
e
n
t
/

A
Time/sec
A
C
u
r
r
e
n
t
/

A
Time/sec
0.000 0.002 0.004 0.006 0.008 0.010 0.012 0.014
5
10
15
20
25
C/ M
R=0.996
B
Fig. 8. (A) The amperometric response of CDtrode for the successive addition of 0.50mmol/L glucose in 0.1mol/L PBS (pH 6.5) at 0.50V under gently stirring. The CDtrode
area was 3mm3mm. (B) The corresponding calibration curve for glucose.
3.6. Amperometric detection of glucose by the CDtrode
The amperometric response measurements of CDtrode were
performed for the successive addition of 0.50mmol/L glucose in
0.1mol/L PBS (pH 6.5) at 0.50V under gentle stirring. Fig. 8(A)
shows a typical currenttime plot for the CDtrode electrode upon
consecutive additions of glucose. The response current increased
with successive additions of glucose. The inset plot displays the
response currents reaching a steady-state current signal within 1s,
indicating a fast response of the sensor. The response time was
much shorter than other reported glucose sensors [3337], as sum-
marized in Table 1. Fig. 8(B) displays the corresponding calibration
curve for glucose. The linear response range of the biosensor to
glucose was from0.5mmol/L to 13mmol/L and the corresponding
linearity (R) is 0.996. The detection limit is 0.035mmol/L. The limit
of determination is lower than 1.0mmol/L, which is the regular
those of commercialized glucometer sensors [38].
3.7. Anti-interferent ability, repeatability, reproducibility and
stability of the CDtrode
Over the last decades, a number of studies have been conducted
to alleviate the drawbacks of enzymatic glucose sensors. The most
common and serious problem is insufcient stability originated
from the nature of the enzymes (either glucose oxidase (GOx) or
glucose dehydrogenase (GDH)), which is hardly overcome [39]. All
strips of glucometers in sold can be adversely affected by temper-
ature, humidity and light. The strips should be consumed within
3 months from opening the packet. The glucose oxidase is inex-
pensive but requires oxygen as a cosubstrate. Consequently, as
oxygen is depleted in the sample, performance decreases, whether
one is monitoring oxygen depletion, or hydrogen peroxide produc-
tion. A number of variables can inuence the reliability of the test
results, including hematocrit, hypoxemia and hypotension. This
sensor avoided the independence of oxygen. Glucose dehydroge-
nase is oxygen independent, and has the added attraction of being
Table 1
The response time compared with different glucose sensors.
Electrode modier Response time (s) Reference
GOD/ZnO-NPs/GCE <4 Ali et al. [33]
GOD/NLDH/CHT/GCE <5 Xu et al. [34]
CoONRs/FTO 2040 Kung et al. [35]
Cu-NPs/ZnO/GCE <3 Kumar et al. [36]
NiHCF/GCE <4 Wang et al. [37]
The proposed CDtrode <1
a well-established probe for monitoring biochemical reactions. The
drawback is that the cofactors are relatively expensive and unsta-
ble [40]. Also, the use of pyrroloquinoline quinone (PQQ) glucose
dehydrogenase may be subjected to interference from a variety
of substances, namely maltose, icodextrin, galactose, xylose. [41].
Ascorbic acid (AA) and uric acid (UA), which normally coexist with
glucose in human blood, are well-known main interferents to the
amperometric responseof glucose. Toevaluatetheselectivityof the
proposed biosensor, AA and UA were examined. Considering that
the concentration of glucose in the healthy human blood is more
than 30 times that of AAand UA[42], 1mmol/L glucose, 0.1mmol/L
AA and 0.1mmol/L UA were added to 0.1mmol/L PBS (pH 6.5) for
the amperometric response measurement of the CDtrode. In Fig. 9,
the impact of UA and AA is nearly eliminated. This is because a
negative potential can be avoided by the interference of AA and
UA. Furthermore, some main coexist ions in human blood (Na
+
, K
+
,
NH
3
+
, Ca
2+
, Fe
2+
, Cl

, PO
4
3
), maltose, icodextrin, galactose, and
xylose were also been examined, and the effects could be ignored.
The results indicated high selectivity of our CDtrode. Therefore, the
sensor can be used for blood glucose detection effectively.
The response reproducibility of six CDtrodes, prepared under
the same electrode area and in optimumconditions, was estimated
in0.1mol/LPBS(pH6.5) at 0.50Vbytheresponseto1mmol/Lglu-
cose, and yielded a mean current response of 11.1AmM
1
cm
2
with a relative standard deviation (RSD) of 3.7%. The repeatability
0 100 200 300 400 500 600 700 800
1.6
1.8
2.0
2.2
2.4
Glucose
C
u
r
r
e
n
t
/

A
Time/sec
Glucose AA UA
Fig. 9. Currenttime curve recorded at the glucose biosensor for addition of
1 mmol/L glucose, 0.1mmol/L ascorbic acid, and 0.1mmol/L uric acid in 0.1mol/L
PBS (pH 6.5) at 0.50V under gently stirring. The CDtrode area is 3mm3mm.
560 Y. Chen et al. / Sensors and Actuators B 177 (2013) 555561
Table 2
The determination results of glucose in human blood samples.
Sample Glucose concentration (n=6) (mM) Added (mM) Found (mM) RSD% (n=6) Recovery%
1 4.26
3.00 2.87
3.2
95.7
4.00 3.89 97.2
5.00 4.91 98.2
2 3.17
3.00 3.03
3.9
101.3
4.00 3.92 98.0
5.00 4.89 97.8
Table 3
Comparison between the values obtained in the hospital and those obtained by using present sensor for the determination of glucose in human blood samples.
Sample number Determined in the hospital (mM) Determined by our biosensor (mM) Bias (mM)
1 4.46 4.72 +0.26
2 5.39 5.74 +0.35
3 5.73 5.55 0.18
4 6.47 6.18 0.29
5 7.15 7.51 +0.36
of the determination was investigated at 0.50V and 25

C in
0.10mol/L PBS containing 1mmol/L glucose, which yielded a rela-
tive standarddeviationof 4.8%for six continuous determinations of
the same sample by using one proposed electrode. The results indi-
cate that the CDtrode has good reproducibility and repeatability.
Though manufacturers often provide meters at no cost to induce
use of the protable test strips, the consumer cost of each dispos-
able glucose striprangedfromabout $0.35to$1.00. Inour work, the
price of the used recordable compact disc with silver lmis about
$0.2 in China, and the recordable compact disc can provide the sen-
sor materials for more than 100 CDtrodes. The present sensor can
be used repeatedly according to acceptable results of the repeata-
bility test, which suggests that the costs of glucose detections will
be low.
The CDtrodes had to be stored in sealed bags in dry environ-
ments at normal temperature. Their long-termstability was tested
for 4months. The measurement results showthat the response cur-
rent only decreases by 3.2%after 4 months, whichindicates that the
CDtrode is considerably stable.
3.8. Detection of glucose in human blood samples
The sensor was used to determine the glucose in human blood
samples. Blood samples were obtained fromhealthy humans com-
plied with fasting blood test requirements. 15L blood and 15L
0.1mol/L PBS with two micropipettes were dropped on the surface
of the present sensor, respectively. And then, the mixture sam-
ple solution was mixed well in a supersonic generator with 5s.
And then the amperometric response measurements were per-
formed under the optimum conditions at an applied potential of
0.50V. The results of glucose concentrations in blood samples are
listed in Table 2. Recoveries in blood samples were from 95.7% to
101.3%.
Accuracy tests were performed in one hospital by healthcare
professionals and diabetic patients. The glucose concentrations
in fresh human blood samples obtained from our experiments
were compared with those measured by the hospital with YSI
Model 2300 Glucose Analyzer (YellowSprings Instruments, Yellow
Springs, OH). The YSI analyzer uses a GO based method to mea-
sure glucose. The results were listed in Table 3. The bias for each
sample is less than 0.4mM. Within the medical community, home
blood glucose meters are considered clinically accurate if the result
is within 20% of what a lab test would indicate [43]. This compar-
ison clearly shows that our results agree satisfactorily with those
obtained in the hospital.
4. Conclusions
We have developed a non-enzymatic glucose sensor based on
recordable CDs. The maximum current response for the glucose
electrode has been observed at pH 6.5, with a potential 0.50V
in phosphate buffer solution. The response of the proposed elec-
trode to glucose concentrations presented a good linearity over
the range of 0.513mmol/L. The study offered an easy way for the
determination of glucose in human blood directly, and it also pro-
vided an approach to recycle waste CDs. The current response time
for a steady-state current was within 1s. There was no substantial
change in current response in the presence of normal physiolog-
ical concentrations of interferents (AA and UA) for the CDtrode.
The applicability of the method for the determination of glucose
in human blood was demonstrated. As a non-enzymatic sensor,
the analytical results were satisfactory for the direct detection of
glucose in human blood. The newly developed non-enzymatic glu-
cose sensor shows a number of excellent characteristics suchas low
cost, fast response, acceptable sensitivity, reproducibility, selectiv-
ity, and long-time stability. Compared with the existing analysis
using sensors of commercialized glucose meters, the present bio-
chemical analysis of the novel amperometric sensor has to needthe
PBS as the supporting electrolyte. For the probable commercializa-
tion, we will attempt to design a necessary kit which contains PBS
with a function of volumetric sampling. Further researches will be
required for the commercialization of this sensor.
Acknowledgements
The work was supported by the National Natural Science Foun-
dation of China (Grant No. 20975091, 21075107), a project funded
by the Priority Academic Program Development of Jiangsu Higher
Education Institutions (PAPD), and the Innovation Program of
JiangsuProvincial EducationDepartment for Postgraduate students
(2011).
References
[1] S.S. Mahshid, S. Mahshid, A. Dolati, Template-based electrodeposition of Pt/Ni
nanowires and its catalytic activity towards glucose oxidation, Electrochimica
Acta 58 (2011) 551555.
[2] J. Wang, Electrochemical glucose biosensors, Chemical Reviews 108 (2008)
814825.
[3] K.M. El Khatib, R.M. Abdel Hameed, Development of Cu
2
O/CarbonVulcanXC-72
as non-enzymatic sensor for glucose determination, Biosensors and Bioelec-
tronics 26 (2011) 35423548.
Y. Chen et al. / Sensors and Actuators B 177 (2013) 555561 561
[4] A.C. Ayupe de Oliveira, V.C. Assis, M.A. Costa Matos, R.C. Matos, Flow-injection
systemwith glucose oxidase immobilized on a tubular reactor for determina-
tion of glucose in blood samples, Analytica Chimica Acta 535 (2005) 213217.
[5] B.S. Der, J.D. Dattelbaum, Construction of a reagentless glucose biosensor using
molecular exciton luminescence, Analytical Biochemistry 375 (2008) 132140.
[6] M. Pleitez, H.V. Lilienfeld-Toal, W. Mntele, Infrared spectroscopic analysis of
humaninterstitial uidinvitro andinvivo using FT-IRspectroscopy andpulsed
quantum cascade lasers (QCL): establishing a new approach to non invasive
glucose measurement, Spectrochimica Acta Part A 85 (2012) 6165.
[7] H.H. Zhou, H. Chen, S.L. Luo, Preparation and bioelectrochemical responses of
the poly(m-phenylenediamine) glucose oxidase electrode, Sensors and Actua-
tors B 101 (2004) 224230.
[8] Y. Liu, Z.Y. Chu, Y.N. Zhang, W.Q. Jin, Amperometric glucose biosensor with
high sensitivity based on self-assembled Prussian Blue modied electrode,
Electrochimica Acta 54 (2009) 74907494.
[9] D.W. Pan, J.H. Chen, S.Z. Yao, L.H. Nie, J.J. Xia, W.Y. Tao, Amperometric glucose
biosensor based on immobilization of glucose oxidase in electropolymerized
o-aminophenol lmat copper-modied gold electrode, Sensors and Actuators
B 104 (2005) 6874.
[10] A. Safavi, N. Maleki, E. Farjami, Fabrication of a glucose sensor based on a novel
nanocomposite electrode, Biosensors and Bioelectronics 24 (2009) 16551660.
[11] D. Rathod, C. Dickinson, D. Egan, Platinum nanoparticle decoration of carbon
materials with applications in non-enzymatic glucose sensing, Sensors and
Actuators B 143 (2010) 547554.
[12] S. Cherevko, C.H. Chung, Gold nanowire array electrode for non-enzymatic
voltammetric and amperometric glucose detection, Sensors and Actuators B
142 (2009) 216223.
[13] S. Cherevko, C.H. Chung, The porous CuOelectrode fabricatedby hydrogenbub-
ble evolution and its application to highly sensitive non-enzymatic glucose
detection, Talanta 80 (2010) 13711377.
[14] Y. Ding, Y. Wang, L. Su, M. Bellagamba, H. Zhang, Y. Lei, Electrospun Co
3
O
4
nanobers for sensitive and selective glucose detection, Biosensors and Bio-
electronics 26 (2010) 542548.
[15] Y. Mu, D.L. Jia, Y.Y. He, Nano nickel oxide modied non-enzymatic glucose sen-
sors with enhanced sensitivity through an electrochemical process strategy at
high potential, Biosensors and Bioelectronics 26 (2011) 29482952.
[16] F. Xiao, F.Q. Zhao, L.Z. Deng, B.Z. Zeng, High electrocatalytic effect of PtAuPd
ternary alloy nanoparticles electrodeposited on mercapto ionic liquid lm,
Electrochemistry Communications 12 (2010) 620623.
[17] J.P. Wang, D.F. Thomas, A.C. Chen, Nonenzymatic electrochemical glucose
sensor based on nanoporous PtPb networks, Analytical Chemistry 80 (2008)
9971004.
[18] M.Q. Guo, R. Wang, X.H. Xu, Electrosynthesis of pinecone-shaped PtPb nano-
structures based on the application in glucose detection, Materials Science and
Engineering C 31 (2011) 17001705.
[19] H. Zhu, X.Q. Lu, M.X. Li, Nonenzymatic glucose voltammetric sensor based on
gold nanoparticles/carbon nanotubes/ionic liquid nanocomposite, Talanta 79
(2009) 14461453.
[20] S.M. Usman Ali, O. Nur, M. Willander, B. Danielsson, A fast and sensitive
potentiometric glucose microsensor based on glucose oxidase coated ZnO
nanowires grown on a thin silver wire, Sensors and Actuators B 145 (2010)
869874.
[21] M.J. Ba nuls, F. Garca-Pi nn, R. Puchades, . Maquieira, Chemical derivatiza-
tion of compact disc polycarbonate surfaces for SNPs detection, Bioconjugate
Chemistry 19 (2008) 665672.
[22] S. Morais, J. Carrascosa, D. Mira, R. Puchades, . Maquieira, Microimmuno-
analysis on standard compact discs to determine low abundant compounds,
Analytical Chemistry 79 (2007) 76287635.
[23] W.A. Challener, R.R. Ollmann, K.K. Kam, Asurface plasmonresonancegas sensor
in a compact disc format, Sensors and Actuators B 56 (1999) 254258.
[24] J. Tamarit-Lpez, S. Morais, R. Puchades, . Maquieira, Use of polystyrene spin-
coated compact discs for microimmunoassaying, Analytica Chimica Acta 609
(2008) 120130.
[25] I. Alexandre, Y. Houbion, J. Collet, S. Hamels, J. Demarteau, J.L. Gala, J. Remacle,
Compact disc with both numeric and genomic information as DNA microarray
platform, BioTechniques 33 (2002) 435439.
[26] R.A.A. Munoz, R.C. Matos, L. Angnes, Gold electrodes from compact discs
modied with platinum for amperometric determination of ascorbic acid in
pharmaceutical formulations, Talanta 55 (2001) 855860.
[27] M.C. Radulescu, A.F. Danet, Mercury determination in sh samples by
chronopotentiometric stripping analysis using gold electrodes prepared from
recordable CDs, Sensors 8 (2008) 71577171.
[28] L. Angnes, E.M. Richter, M.A. Augelli, G.H. Kume, Gold electrodes fromrecord-
able CDs, Analytical Chemistry 72 (2000) 55035506.
[29] C. Ho, D.M. Soolaman, H.Z. Yu, 2004 Fred Beamish Award Lectureanalytical-
materials chemistry on old CDsbeyond self-assembly, Canadian Journal of
Chemistry 83 (2005) 403412.
[30] E.M. Richter, M.A. Augelli, G.H. Kume, R.N. Mioshi, L. Angnes, Gold electrodes
fromrecordable CDs for mercury quantication by owinjection analysis, Fre-
senius Journal of Chemistry 366 (2000) 444448.
[31] H.F. Cui, J.S. Ye, W.D. Zhang, C.M. Li, J.H.T. Luong, F.S. Sheu, Selective and
sensitive electrochemical detection of glucose in neutral solution using
platinumlead alloy nanoparticle/carbon nanotube nanocomposites, Analytica
Chimica Acta 594 (2007) 175183.
[32] H.P. Huang, J.J. Zhu, Preparation of novel carbon-based nanomaterial of
graphene and its applications electrochemistry, Chinese Journal of Analytical
Chemistry 39 (2011) 963971.
[33] S.M.U. Ali, O.N.M. Willander, B. Danielsson, A fast and sensitive potentio-
metric glucose microsensor based on glucose oxidase coated ZnO nanowires
grown on a thin silver wire, Sensors and Actuators B: Chemical 145 (2010)
869874.
[34] Y.H. Xu, X.J. Liu, Y.P. Ding, L.Q. Luo, Y.L. Wang, Y. Zhang, Y.J. Xu, Preparation
andelectrochemical investigationof a nano-structuredmaterial Ni
2+
/MgFe lay-
ered double hydroxide as a glucose biosensor, Applied Clay Science 52 (2011)
322327.
[35] C.W. Kung, C.Y. Lin, Y.H. Lai, R. Vittal, K.C. Ho, Cobalt oxide acicular nanorods
with high sensitivity for the non-enzymatic detection of glucose, Biosensors
and Bioelectronics 27 (2011) 125131.
[36] S.A. Kumar, H.W. Cheng, S.M. Chen, S.F. Wang, Preparation and characteriza-
tion of copper nanoparticles/zinc oxide composite modied electrode and its
application to glucose sensing, Materials Science and Engineering C 30 (2010)
8691.
[37] X.Y. Wang, Y. Zhang, C.E. Banks, Q.Y. Chen, X.B. Ji, Non-enzymatic
amperometric glucose biosensor based on nickel hexacyanoferrate
nanoparticle lm modied electrodes, Colloids and Surfaces B 78 (2010)
363366.
[38] K.E. Toghill, R.G. Compton, Electrochemical non-enzymatic glucose sensors: a
perspective andanevaluation, International Journal of Electrochemical Science
5 (2010) 12461301.
[39] S. Park, H. Boo, T.D. Chung, Electrochemical non-enzymatic glucose sensors,
Analytica Chimica Acta 556 (2006) 4657.
[40] J.D. Newman, A.P.F. Turner, Home blood glucose biosensors: a commercial per-
spective, Biosensors and Bioelectronics 20 (2005) 24352453.
[41] M. Montagnanaa, M. Caputob, D. Giavarinac, G. Lippi, Overview on self-
monitoring of blood glucose, Clinica Chimica Acta 402 (2009) 713.
[42] W. Wang, Z.Y. Li, W. Zheng, J. Yang, H. Zhang, C. Wang, Electrospun palladium
(IV)-doped copper oxide composite nanobers for non-enzymatic glucose sen-
sors, Electrochemistry Communications 11 (2009) 18111814.
[43] T.M. Gross, B.W. Bode, D. Einhorn, D.M. Kayne, J.H. Reed, N.H. White, J.J.
Mastrototaro, Performance evaluation of the MiniMed

continuous glucose
monitoring systemduring patient home use, Diabetes Technology and Thera-
peutics 2 (2000) 4956.
Biographies
Yuxing Chen received the B.S. degree fromDezhou University, China, in 2010. Her
work is focusedonthe nonenzymatic glucose sensors andtheir potential application
for blood glucose detection as a postgraduate.
Lin Liu is a postgraduate student in Yangzhou University. Her research eld is elec-
trochemical sensors in health care.
Meirong Wang is doing research for her Master degree in Yangzhou University.
Her work is focused on the electrochemical sensors and synthesis of polymers by
electrochemical methods.
ChengyinWangis aprofessor inanalytical chemistryat theCollegeof Chemistryand
Chemical Engineering, YangzhouUniversity. He receivedhis Ph.D. degree inphysical
chemistry fromYangzhou University in 2007. His major research interests include
biosensor and chemical sensor, nanomaterials and nanoelectrode, chromatography.
Xiaoya Hu is a professor in analytical chemistry at the College of Chemistry and
Chemical Engineering, Yangzhou University. He received his Ph.D. degree in ana-
lytical chemistry fromNanjing University in 1999. His main research is focused on
sensors and nanotechnology.
Guoxiu Wang received his Ph.D. degree in Materials Science and Engineering
in 2001 from University of Wollongong, Australia. He is currently working as a
Professor at School of Chemistry and Forensic Science, University of Technology,
Sydney, Australia, and a director of Centre for Clean Energy Technology. His major
research interests include nanostructured functional materials, materials chem-
istry in energy storage and conversion, and development of chemical and biological
sensors.

Vous aimerez peut-être aussi