Transfer-free CVD graphene for highly sensitive glucose sensors

doi:10.1016/j.jmst.2019.07.039

Abstract

Abstract:

Chemical vapor deposition (CVD) graphene film is a promising electrode-modifying material for fabricating high-performance glucose sensor due to its high electrical conductivity and two-dimensional structure over large area. However, the use of typical metal-based CVD graphene suffers from the residue contamination of polymer transfer-support and heavy metal ions. In this work, we directly grew few-layer graphene on the SiO₂/Si substrate without transfer process and then fabricated graphene-based glucose sensors by sequentially immobilizing glucose oxidase and depositing Nafion layer on its surface that was functionalized by oxygen-plasma treatment. Our transfer- and metal-free process shows distinct advantage over the common metal-CVD method in improving the electrochemical performance by eliminating the contamination of transfer-residue. Thus-obtained glucose sensor shows a high sensitivity (16.16 μA mM^-1 cm^-2) with a detection limit of 124.19 μM. This method is simple and promising for the development of highly sensitive glucose sensors.

Key words: Graphene, Chemical vapor deposition, Transfer-free, Oxygen-plasma treatment, Glucose sensor

Shijing Wei, Yabin Hao, Zhe Ying, Chuan Xu, Qinwei Wei, Sen Xue, Hui-Ming Cheng, Wencai Ren, Lai-Peng Ma, You Zeng. Transfer-free CVD graphene for highly sensitive glucose sensors[J]. J. Mater. Sci. Technol., 2020, 37: 71-76.

Figures/Tables 6

Fig. 1. Schematic fabrication process of the graphene sensor. First, few-layer graphene is directly grown on a SiO2/Si substrate (a) by metal-free thermal CVD to form the G/SiO2/Si sample (b). The Nafion/GOx/OPG/SiO2/Si electrode is then formed by bonding the sample with copper wire (c), followed by sequential treatment with oxygen plasma (d), coating with GOx (e) and Nafion layers (f).

Fig. 2. Characterization of pristine G/SiO2/Si and OPG (after the oxygen-plasma treatment for 20?s): (a) Raman spectra; (b) optical transmittance spectra (transferred on quartz); AFM images (on SiO2/Si substrates) of the pristine graphene (c) and OPG (d). The insets of (b) show the corresponding optical micrographs.

Fig. 3. Contact angle measurements of pristine graphene and OPG. Pristine graphene: θc?=?90°; OPG: θc?=?26°. Inset: Photographs of wetting properties of pristine graphene (left) and OPG (right).

Fig. 4. (a) Full XPS spectra comparison of pristine graphene and OPG, XPS C1s spectra of (b) the pristine graphene and (c) OPG treated for 20?s and (d) percentage of integrated peak area ratios of the resolved C1s peaks in pristine graphene and OPG.

Fig. 5. (a) Cyclic voltammograms of SiO2/Si, G/SiO2/Si, OPG/SiO2/Si and Nafion/GOx/OPG/SiO2/Si modified electrodes in 0.1?M PBS (pH?=?7) saturated with N2 at a scan rate of 100?mV s-1; (b) Cyclic voltammograms at various scan rates from 10, 25, 50, 100, 150, 200 and 250 to 300?mV s-1, respectively. Inset: plot of peak current versus scan rate; (c) Amperometric response at -0.5?V for Nafion/GOx/OPG/SiO2/Si electrode with dropwise addition of glucose concentrations of 400 μM to 2000 μM in O2 saturated 0.1?M PBS. (d) Linear regression curve of current versus glucose concentrations.

Table 1 Performance comparison of the Nafion/GOx/OPG/SiO2/Si electrode with other electrodes of glucose sensors.

Modified electrodes	Sensitivity (μA mM^-1?cm^-2)	LOD (μM)	Ref.
Nafion/GOx/OPG/SiO₂/Si	16.16	124.19	This work
GOx/OPG/SiO₂/Si	0.118	52.6	[21]
GOx/AuNPs/CVD-G/GCE	0.003	4	[22]
Ni(OH)₂/3DGF	2.65	0.34	[36]
AuNPs-FLG/ITO	0.195	1	[37]
AuNPs-NG/ITO	0.25	12	[38]
Nafion/GOx/MnO₂-RGO/GCE	3.3	10	[39]
GOx/AuNPs/RGO-IL/GCE	0.16	130	[40]
GOx/RGO/AuE	21.9	40	[9]
GOx/RGO/GCE	110	10	[10]
GOx/RGO/PGE	278.4	0.61	[11]

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