Study of Electrochemical Non-enzyme Glucose Sensor Based on Cu(Ⅱ)Co(Ⅱ) Bimetallic Carbon Nanosheets

doi:10.19894/j.issn.1000-0518.220099

Chinese Journal of Applied Chemistry ›› 2022, Vol. 39 ›› Issue (12): 1891-1902.DOI: 10.19894/j.issn.1000-0518.220099

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Study of Electrochemical Non-enzyme Glucose Sensor Based on Cu(Ⅱ)Co(Ⅱ) Bimetallic Carbon Nanosheets

Xiao-Mei HUANG¹^,²^,³(), Xiang DENG¹^,², Lang-Man XING¹, Wei CHEN¹, Li SUN¹, Xiao-Yu ZHU¹

^1.Department of Chemistry and Chemical Engineering，Sichuan University of Arts and Science，Dazhou 635000，China
^2.Key Laboratory of Exploitation and Study of Distinctive Plants in Education Department of Sichuan Province，Dazhou 635000，China
^3.Key Laboratory of Green Chemistry of Sichuan Institutes of Higher Education，Zigong 643000，China

Received:2022-04-01 Accepted:2022-08-31 Published:2022-12-01 Online:2022-12-13
Contact: Xiao-Mei HUANG
About author:huangxm917@163.com
Supported by:
the Scientific Research Fund of the Sichuan Provincial Science and Technology Department(2019YJ0307);the Key Laboratory of Exploitation and Study of Distinctive Plants in Education Department of Sichuan Province(TSZW2005);the Opening Project of Key Laboratory of Green Chemistry of Sichuan Institutes of Higher Education(LYJ1802);Dazhou Municipal Science Project of Technology Bureau Application Foundation(18YYJC0002);the National University Innovation and Entrepreneurship Training Program(202110644011);the Scientific Research Program for College Students of Sichuan University of Arts and Sciences in 2021(X2021Z021)

Abstract

Abstract:

CuCo-MOF nanofibers are synthesized by one-step solvent blending process at room temperature. Then CuCo-MOF nanofibers are used as the precursors， carbon nanosheets （Cu（Ⅱ）Co（Ⅱ）@C） uniformly loaded with nano-sized copper oxide and cobalt oxide are obtained by calcination at high temperature in air. Cu（Ⅱ）Co（Ⅱ）@C is modified on the glassy carbon electrode to directly catalyze glucose in alkaline solution. Because CuO and CoO are uniformly and firmly embedded on the carbon nanosheets， the agglomeration of catalyst is prevented， which greatly improves the specific surface area， and increases the catalytic active site. Meanwhile， due to the synergistic effect of copper and cobalt bimetals in the carbon nanosheet material， the enzyme free glucose sensor has excellent electrical conductivity and excellent catalytic performance. The detection range of the non-enzymatic electrochemical glucose sensors for glucose is 0.03 μmol/L~13.6 mmol/L， the detection limit is 0.01 μmol/L （S/N=3）， and the sensitivity is 10.56 mA·L/（cm²·mmol）. In addition， the non-enzyme sensor also has good anti-interference and high stability.

Key words: Metal organic frameworks, Cu（Ⅱ）CO（Ⅱ） bimetallic carbon based nanosheets, Non-enzymatic glucose sensors, Synergistic effect

CLC Number:

O646

Xiao-Mei HUANG, Xiang DENG, Lang-Man XING, Wei CHEN, Li SUN, Xiao-Yu ZHU. Study of Electrochemical Non-enzyme Glucose Sensor Based on Cu(Ⅱ)Co(Ⅱ) Bimetallic Carbon Nanosheets[J]. Chinese Journal of Applied Chemistry, 2022, 39(12): 1891-1902.

Figures/Tables 8

Fig.1 （A） Schematic diagram of preparation of Cu（Ⅱ）Co（Ⅱ）@C；（B） Construction process of non-enzymatic glucose sensor

Fig.2 SEM images of CuCo-MOF （A） and Cu（Ⅱ）Co（Ⅱ）@C （B）， in the red circle of figure B， there are Cu （Ⅱ） and Co （Ⅱ） nanoparticles；（C） and （D） TEM images of Cu（Ⅱ）Co（Ⅱ）@C；（E） Cyclic voltammetry （CV） curves of bare GCE（a） and Cu（Ⅱ）Co（Ⅱ）@C/GCE（b） in 0.10 mol/L NaOH solution

Fig.3 （A） XRD pattern of Cu（Ⅱ）Co（Ⅱ）@C；（B） XPS spectra of Cu（Ⅱ）Co（Ⅱ）@C full scan；（C） and （D） are high-resolution XPS spectra of Cu2p and Co2p， respectively

Fig.4 （A） CV curves of different materials in 0.10 mol/L NaOH solution containing 0.50 mmol/L glucose；` （B） The amperometric response of the current with time when an equal concentration of glucose solution is continuously added to 5 mL of 0.10 mol/L NaOH solution under stirring conditions. （a） Cu（Ⅱ）@C，（b） CuCo-MOF，（c） Cu（Ⅱ）Co（Ⅱ）@C；（C） Catalytic activity of Cu（Ⅱ）Co（Ⅱ）@C with six different n（Cu）∶ n（Co） to glucose；（D） Catalytic activity of Cu（Ⅱ）Co（Ⅱ）@C/GCE to glucose at different potentials；（E） CV curves of Cu（Ⅱ）Co（Ⅱ）@C/GCE at different scan rates from 10 to 300 mV/s in 0.10 mol/L NaOH solution containing 0.50 mmol/L glucose；（F） Linear plots of reduction peak and oxidation peak current vs. the square root of the scan rate. Supporting electrolyte is 0.10 mol/L NaOH solution

Fig. 5 （A） CV curves of Cu(Ⅱ)Co(Ⅱ)@C/GCE in 0.10 mol/L NaOH solution without glucose and with 0.50 mmol/L glucose；（B） Reaction mechanism diagram；（C） Amperometric response of Cu（Ⅱ）Co（Ⅱ）@C/GCE at 0.45 V by continuously injecting glucose；（D） The corresponding calibration plot of （C）， error bars are the standard deviation of 3 measurements

Table 1 Comparison of amperometric responses of the modified electrodes to glucose

传感器	检测范围	灵敏度	检测限	参考文献
Sensor	Linear range	Sensitivity/（mA·L·cm^－2·mmol^－1）	LOD/（μmol·L^－1）	Ref.
Pt-Ni NPs-MWCNTs/GCE	7.0~16.0 mmol/L	0.57	230	［46］
Cu@HHNs/GCE	5 μmol/L~3 mmol/L	1.59	1.97	［47］
Au@Ni/C/GCE	0.5~10 mmol/L	0.023	15.7	［48］
M-BDC MOF/GCE	0.01~0.8 mmol/L	0.64	6.68	［49］
NiCo NSs/GNR-GCE	5 μmol/L~0.8 mmol/L	0.34	0.6	［50］
Cu（Ⅱ）Co（Ⅱ）@C/GCE	0.03 μmol/L~13.6 mmol/L	10.56	0.01	This work

Fig 6 （A） Effects of Cu on glucose detection in 0.10 mol/L NaOH solution with 0.20 mmol/L fructose， dopamine （DA）， ascorbic acid （AA）， uric acid （UA）， lactose， sucrose， galactose and paracetamol， respectively；（B） Stability of non-enzymatic glucose biosensors with scanning speed of 50 mV/s in 0.10 mol/L NaOH solution containing 0.50 mmol/L glucose

Table 2 Appearance of the biosensor for determination the recovery of glucose

样品号	血清样品	葡萄糖加入量	实验值	医院测定值	回收率	相对标准偏差
Sample No.	c（Original）/（μmol·L^－1）	c（Added）/（μmol·L^－1）	Found ^a / （μmol·L^－1）	Determined by hospital ^b /（μmol·L^－1）	Recovery/%	RSD% （n=3）
1	50	10	61.23±3.8	60.46±3.2	102.1	4.2
2	100	20	122.1±3.2	123.24±2.6	101.7	3.8
3	200	50	245.6±8.1	247.1±5.4	98.2	2.4
4	400	100	484.5±18.6	479.5±19.3	96.3	2.9

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Study of Electrochemical Non-enzyme Glucose Sensor Based on Cu(Ⅱ)Co(Ⅱ) Bimetallic Carbon Nanosheets

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