Sandwich structure confined gold as highly sensitive and stable electrochemical non-enzymatic glucose sensor with low oxidation potential

doi:10.1016/j.jmst.2022.01.014

Abstract

Abstract:

The preparation of highly sensitive and stable non-enzymatic glucose sensors is critical to the prevention and treatment of diabetes. Fe₃O₄@Au@CoFe-LDH is prepared through a spontaneous galvanic displacement reaction. A series of structural characterizations testify the successful formation of Fe₃O₄@Au@CoFe-LDH electrocatalyst, with the Au intercalating between Fe₃O₄ and LDH to form the sandwich structure. Cyclic voltammetry tests indicate that Au is responsible for the electrocatalytic oxidation of glucose. The characterizations of the electrochemical sensor for glucose detection indicate that Fe₃O₄@Au@CoFe-LDH possesses high sensitivity of 6342 μA mM^-1 cm^-2, with an extremely low oxidation potential of 0.82 V vs. RHE. Even with the high glucose concentration of 15 mM, the sensitivity remains at 4359 μA mM^-1 cm^-2. Due to the broad linear detection range (0.0375 to 15.64 mM) and the low limit of detection (12.7 μM), Fe₃O₄@Au@CoFe-LDH is applicable towards practical application. Thanks to the sandwich structure, which confines the Au in between Fe₃O₄ and CoFe-LDH, the Fe₃O₄@Au@CoFe-LDH glucose sensor shows high long-term stability and satisfactory selectivity. The successful synthesis of the sandwich-structured Fe₃O₄@Au@CoFe-LDH provides a new conception for the design of highly sensitive and stable non-enzymatic glucose electrodes.

Key words: Electrochemical glucose sensors, Non-enzymatic, Sandwich structure, Au

Fengchao Sun, Xingzhao Wang, Zihan You, Hanhan Xia, Shutao Wang, Cuiping Jia, Yan Zhou, Jun Zhang. Sandwich structure confined gold as highly sensitive and stable electrochemical non-enzymatic glucose sensor with low oxidation potential[J]. J. Mater. Sci. Technol., 2022, 123: 113-122.

Figures/Tables 9

Scheme 1. Designed synthesis method of Fe3O4@Au@CoFe-LDH.

Fig. 1. (a) XRD patterns of CoFe-LDH and Fe3O4@Au@CoFe-LDH and (b) the powder samples peeled off from iron foams. (c) Raman spectra of CoFe-LDH and Fe3O4@Au@CoFe-LDH. (d) SEM image, (e) TEM image, and (f) HRTEM image of CoFe-LDH. (g) SEM image, (h) TEM image, and (i) HRTEM image of Fe3O4@Au@CoFe-LDH.

Fig. 2. XPS spectra of CoFe-LDH and Fe3O4@Au@CoFe-LDH: (a) the survey scan spectra, (b) Co 2p, (c) Fe 2p and (d) Au 4f regions.

Fig. 3. (a) TEM, (b) HRTEM images of Fe3O4@Au@CoFe-LDH-1000, and (c, d) the corresponding diffraction pattern measured with FFT at different positions.

Fig. 4. Cyclic voltammetry curves of (a) CoFe-LDH and (b) Fe3O4@Au@CoFe-LDH in 1.0 M KOH with and without 50 mM glucose with the scan rate of 50 mV s - 1. (c) Cyclic voltammetry curves of Fe3O4@Au@CoFe-LDH in 1.0 M KOH at different scan rates of 50, 100, 150, 200, and 250 mV s - 1 and (d) the corresponding plots of the peak current vs. the square root of scan rates at about 0.17 and 0.4 V vs. Hg/HgO.

Fig. 5. (a) Chronoamperometry response of Fe3O4@Au@CoFe-LDH toward glucose in 1.0 M KOH with continuous glucose at -0.1 V vs. Hg/HgO. (b) Corresponding linear fitting between glucose concentration and current density. (c) Sensitivity of Fe3O4@Au@CoFe-LDH at the various test potentials. (d) Sensing performance comparison of this work and other previous works in test potential and sensitivity.

Fig. 6. (a) Selectivity test of Fe3O4@Au@CoFe-LDH in 1.0 M KOH with 10 μM glucose concentration and 0.33 μM interference concentration at -0.1 V vs. Hg/HgO. The interferences are uric acid (UA), sodium chloride (NaCl), galactose (Gal), fructose (Fru), ascorbic acid (AA), and 4-acetamidophenol (AP). (b) Change of current density of glucose and the interfering species in selectivity test. (c) Stability test of Fe3O4@Au@CoFe-LDH in 1.0 M KOH at -0.1 V vs. Hg/HgO.

Fig. 7. Cyclic voltammetry curves of (a) Fe3O4@CoFe-LDH and (b) Au NPs/CP in 1.0 M KOH with and without 50 mM glucose with the scan rate of 50 mV s - 1. (c) Stability test of CoFe-LDH and Fe3O4@CoFe-LDH in 1.0 M KOH with 500 mM glucose at the current density of 100 mA cm-2.

Fig. 8. Schematic illustration for electrocatalytic oxidation of glucose on Fe3O4@Au@CoFe-LDH sensor.

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