A graphene-laminated electrode with high glucose oxidase loading for highly-sensitive glucose detection

doi:10.1016/j.jmst.2020.04.070

Abstract

Abstract:

Graphene oxide (GO) has received considerable attention for glucose detection because of high surface area, abundant functional groups, and good biocompatibility. Defects and functional groups of the GO are beneficial to immobilization of glucose oxidase (GOD), but sacrificing electron-transfer capability for highly-sensitive detection. In order to obtain high GOD loading and highly-sensitive detection of biosensors, we first designed and fabricated a graphene-laminated electrode by combining GO and edge-functionalized graphene (FG) layers together onto glassy-carbon electrode. The graphene-laminated electrodes exhibited faster electron transfer rate, higher GOD loading of 3.80 × 10^-9 mol?cm^-2, and higher detection sensitivity of 46.71 μA?mM^-1?cm^-2 than other graphene-based biosensors reported in literature. Such high performance is mainly attributed to the abundant functional groups of GO, high electrical conductivity of FG, and strong interactions between components in the graphene-laminated electrodes. By virtue of their high enzyme loading and highly-sensitive detection, the graphene-laminated electrodes show great potential to be widely used as high-performance biosensors in the field of medical diagnosis.

Key words: Graphene, Laminated structure, Electrode, Glucose detection, Biosensor

Yabin Hao, Minghe Fang, Chuan Xu, Zhe Ying, Han Wang, Rui Zhang, Hui-Ming Cheng, You Zeng. A graphene-laminated electrode with high glucose oxidase loading for highly-sensitive glucose detection[J]. J. Mater. Sci. Technol., 2021, 66: 57-63.

Figures/Tables 8

Fig. 1. Preparation schematic of the graphene-laminated electrode (GCE-RFG-RGO-GOD-CS), including the successive coating of FG, GO, GOD, CS onto GCE surface and the electrochemical reduction treatment.

Fig. 2. (a) XPS survey spectra, (b) oxygen contents, and (c) corresponding chemical composition of the GO, RGO, FG and RFG.

Fig. 3. Nyquist plots of EIS for the bare GCE and graphene-laminated electrodes.

Fig. 4. (a) CV curves and (b) peak currents of the graphene-laminated electrodes.

Fig. 5. (a) CV curves of the graphene-laminated electrodes in PBS solutions with different pH values (scanning rate of 50 mV?s-1), and (b) the dependence of formal potential (E°) on pH value.

Fig. 6. (a) CV curves of the graphene-laminated electrodes in PBS solution (pH = 7) at different scanning rates of 25, 50, 100, 150, 200, 250, and 300 mV?s-1, and (b) the dependence of peak currents on scanning rates.

Table 1 Performance comparison of various graphene-decorated GCEs.

Electrode	Γ (mol˖cm^-2)	Sensitivity (μA∙mM^-1∙cm^-2)	LOD (μM)	Reference
GCE-G-MWCNTs-AuNPs-GOD	2.22 × 10^-10	29.72	4.8	[34]
GCE-G-GOD-CS	1.12 × 10^-9	37.93	20	[52]
GCE-GR-CoPc-GOD	3.77 × 10^-10	5.09	1.6	[54]
GCE-RGO-MnO₂-GOD-Nafion	1.75 × 10^-10	3.3	10	[55]
GCE-RGO-GOD	1.22 × 10^-10	1.85	-	[44]
GCE-RGO-AuNPs-GOD	-	0.16	130	[36]
GCE-RFG-RGO-GOD-CS	3.80 × 10^-9	46.71	79.65	This work

Fig. 7. (a) Amperometric response of the graphene-laminated electrodes with successive addition of glucose into PBS solution, and (b) the dependence of response currents on glucose concentrations.

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