Microsoft Word - 280204-1009.doc/
1 1 1 1,2 1*1,2,3
Using Ionic Liquid to Improve Glucose Sensing Performance of PdAu/graphene Nanocomposite
Electrodes C. H. Wang1, C. H. Yang1, J. W. Wu1, Y. C. Wang1,2, M. T. Lee1, J. K. Chang*1,2,3
Received 30 July 2013; received in revised form 10 January 2014; accepted 16 February 2014
/(PdAu/graphene)
/(Au/graphene)/(Pd/graphene)
///
1-Butyl-1-Methylpyrrolidinium Bis (trifluoromethylsulfonyl) imide (BMP-NTF2)

ABSTRACT
In this study, we synthesize PdAu/graphene nanocomposites by supercritical carbon dioxide (scCO2) for non-enzymatic glucose detection. With the aid of scCO2, which has gas-like diffusivity, extremely low viscosity, and near-zero surface tension, the synthesized nano-sized PdAu particles (approximately 5 nm in diameter) are uniformly distributed on graphene. For comparison, Pd/graphene and Au/graphene are both synthesized using the same process. The PdAu/graphene electrode shows higher current density than Pd/graphene and lower oxidation potential than Au/graphene in detecting glucose. With the incorporation of 1-Butyl-1-Methylpyrrolidinium
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Journal of Chinese Corrosion Engineering, Vol. 28, No. 6, pp. 81 ~ 88 (2014)

1
1 Institute of Materials Science and Engineering, National Central University. 2
2 Department of Chemical and Materials Engineering, National Central University 3
3 Department of Mechanical Engineering, National Central University * jkchang@ncu.edu.tw
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Keywords: PdAu nanoparticle; Graphene; Glucose; Supercritical carbon dioxide; Ionic liquid.
1.

[5-8]




2. 2.1
(graphene nanosheet) modified Staudenmaier [12,13]
5 (Alfa Aesar, with particle size of ~ 70 µm and purity of 99.999%)100
50 50 100 (graphite oxide, GO)
(GO) 5 wt%

2.2 /
Palladium(II)-hexafluoro- acetylacetonate (Pd(hfa)2, Aldrich, 99%)
HAuCl4•3H2O (Aldrich, 98%)
(dimethylamine borane, DMAB, TCI, > 95%)
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100 bar 2
/(PdAu/graphene)/
2.3 2.5 mg 650 µl
(isopropyl alcohol, IPA, TEDIA, > 99.5%)90 µl (5 wt% Nafion, Aldrich)
2
15 µl
BMP-NTf2 7 µL
(7 µL + 8 µL)

(cyclic voltammetry)
(chronoamperometry)
(2θ) 40°46.3° 68.1°
Pd (111)Pd (200) Pd (220)(2θ) 38.2°44.5°64.7° 77.6°
Au (111)Au (200)Au (220) Au (331) PdAu 38.8°44.9° 65.7° PdAu/graphene Pd/graphene
Au/graphene
(λ = 0.15418 nm) Scherrer’s equation
(grain size, D)
15.35.4 4.7 nm 1(b) (111)
d 0.23 nm 0.236 nm
0.234 nm
40 wt% 60 wt%
(a) (b) 1 (a) /(Pd/graphene)/(PdAu/graphene)/(Au/graphene) X
(b) d
Figure 1 (a) X-ray diffraction patterns of Pd/graphene, PdAu/graphene, and Au/graphene. (b) Relationship between Au content and d-spacing of deposited particles.
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(111)
10 mV/s 3(b)
3(a)/ 0.16 V 0.3 V




(a) (b) (c) (d) 2 (a) /(b) /(c) /(d)

Figure 2 Transmission-electron-microscopy (TEM) bright-field images of (a) Pd/graphene, (b) PdAu/graphene and (c) Au/graphene. (d) High-resolution TEM image of a PdAu nanoparticle.
(a) (b) 3 ///(a) 5 mM 0.1 M NaOH (b)
0.1 M NaOH ( 10 mV/s) Figure 3 Cyclic voltammograms of Pd/graphene, PdAu/graphene, and Au/graphene electrodes recorded in 0.1 M
NaOH solution (a) with 5 mM glucose, and (b) without glucose at a potential scan rate of 10 mV/s.
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-0.4 V 0.2 V
0.2 V


(PdOH)



4(b)
z
5
(a) (b) 4 BMPNTf2//BMPNTf2// BMPNTf2// (a) 5 mM
0.1 M NaOH (b) 0.1 M NaOH ( 10 mV/s) Figure 4 Cyclic voltammograms of BMPNTf2/Pd/graphene, BMPNTf2/PdAu/graphene, and BMPNTf2/Au/graphene
electrodes recorded in 0.1 M NaOH solution (a) with 5 mM glucose and (b) without glucose at a potential scan rate of 10 mV/s.
5 ///
BMPNTf2 5 mM
Figure 5 Net response current of Pd/graphene, PdAu/graphene, and Au/graphene electrodes with and without BMPNTf2 incorporation toward sensing of 5 mM glucose.
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/

6(b)
6(b) 1 mM 10 mM
(R2 = 0.99)

7
(a) (b) 6 (a) BMPNTf2// 1, 3, 5, 7.5, 10 mM 0.1 M NaOH
(b)
Figure 6 (a) Cyclic voltammograms of BMPNTf2/PdAu/graphene electrode recorded in 0.1 M NaOH solution with glucose concentrations of 1, 3, 5, 7.5, and 10 mM. (b) Net response current density as function of glucose concentration.
7 -0.12 V BMPNTf2//
5 mM 0.05 mM 5 mM

Figure 7 Amperometric responses of BMPNTf2/PdAu/graphene electrode to successive additions of 5 mM glucose, 0.05 mM ascorbic acid (AA), and then 5 mM glucose at -0.12 V.
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(-0.12 V) 5 mM 0.05 mM
5 mM


BMP-NTf2//


NSC100-2628-E-008-008-MY3
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