NiCl(OH) nanosheet array as a high sensitivity electrochemical sensor for detecting glucose in human serum and saliva
Graphical abstract
Introduction
In today's society, the control and prevention of diseases has attracted the attention of countries around the world. Diabetic mellitus is also a common disease among many diseases [1]. Hyperglycemic patients need to monitor blood glucose concentrations in real time to observe their physical health. Therefore, there are various methods for detecting glucose in the field of analytical detection [2], [3], [4], [5]. Among them, electrochemical sensing has been widely studied for its fast response, high sensitivity, low detection limit, low cost, and easy operation [6], [7]. Since Clark and Lyons pioneered the application of enzyme-based electrochemical sensing [8], enzyme-based electrochemical sensors have attracted widespread attention and research. However, the use of enzyme-based electrochemical sensors has been limited due to the difficulties in enzyme immobilization and susceptibility of the enzyme to environmental influences [9], [10].
In recent decades, more and more researchers have participated in the research team of non-enzymatic glucose sensors. These studies include noble-metal catalysts and transition-metal catalysts. Although the noble-metal catalyst has high catalytic activity, its high spending has affected its widespread application [11], [12], [13], [14]. Therefore, researchers have favored transition metal oxides [15], [16], [17], [18], oxyhydroxides [19], [20], sulfides [21], [22], [23], phosphides [24], [25], [26], nitrides [27], [28], etc. for glucose sensing. Nickel-based materials are widely used in the electrolysis of hydrogen and oxygen evolution reaction [29], [30], [31], and electrocatalytic oxidation of glucose due to their excellent electrocatalytic performance. For example, Wang et al. [32] synthesized nanowires with core-shell structure: IrO2@NiO, to detect glucose and obtained a sensitivity of 1439.4 μA mM−1 cm−2, linear range of 0.005–2.5 mM and detection limit of 0.3 μM. Guo et al [33]. using the synthesized Ni/CdS bifunctional Ti@TiO2 core-shell nanowire for high-performance sensing of glucose, has obtained a higher sensitivity (1136.67 μA mM−1 cm−2), wide linear range (0.005–12 mM), and detection limit of 0.35 μM.
Herein, with anhydrous ethanol and NiCl2·6H2O as raw materials, NiCl(OH) nanosheets were grown in situ on carbon cloth (NiCl(OH) NS/CC) by a simple one-pot hydrothermal process, which has high electrocatalytic activity for oxidizing glucose in 0.1 M NaOH solution. The electrocatalytic oxidation of glucose resulted in a high sensitivity, a wide detection range and a lower detection limit. In addition, in order to verify the practical feasibility of NiCl(OH) NS/CC electrochemical sensor, real human serum samples and saliva was detected with satisfactory results. The test results of our sensor are consistent with the detection results of commercial blood glucose meters, indicating that the electrochemical sensor has good reliability in sensing glucose.
Section snippets
Reagents and materials
All chemical reagents are analytically pure. We classified each reagent according to its use in this experiment as follows: Anhydrous ethanola, NiCl2·6H2Oa and carbon cloth (CC)b as raw materials and substrate for the synthesis of NiCl(OH) NS/CC. Glucose (Glu)a and sodium hydroxide (NaOH)a were used to prepare the test solution and electrolyte, respectively. NaCla, ureac, uric acid (UA)c, lactosec, dopamine (DA)d, fructosec and ascorbic acid (AA)c were used to formulate interferences in
NiCl(OH) NS/CC material characterization
One-pot hydrothermal method was adopted to synthesize NiCl(OH) NS/CC. It has been found that Cl− may interact with Ni(OH)2 through the ligand exchange process, where the hydroxide may form Ni(OH)Cl [35]. The chemical reaction was as follows [36]:NiCl2 + OH− → NiCl(OH) + Cl−NiCl(OH) + OH– → Ni(OH)2 + Cl−
Ethanol was the hydrothermal solvent is absolute, so it tended to generate NiCl(OH). Fig. 1a shows the XRD spectrum of NiCl(OH) and blank carbon cloth. Compared with standard patterns (JCPDS No.
Conclusions
In summary, one-pot synthesis of NiCl(OH) nanosheets was prepared in situ on carbon cloth, which proved to be an outstanding non-enzymatic glucose sensing electrode in alkaline conditions. The i-t response result of the optimal test potential at 0.50 V confirms that the electrochemical sensor has excellent sensing performance, such as: high sensitivity, short response time, wide linear range, nanomolar detection limit, good reproducibility, selectivity and stability. In addition, NiCl(OH) has a
Declaration of Competing Interest
The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
CRediT authorship contribution statement
Qiang Wang: Conceptualization, Methodology, Validation, Investigation, Writing - original draft. Zhipeng Wang: Writing - original draft, Investigation. Qiaoyan Dong: Writing - original draft. Ruoxi Yu: Investigation. Haihong Zhu: Investigation. Zhirong Zou: Supervision, Writing - review & editing. Huimin Yu: Supervision, Writing - review & editing. Ke Huang: Supervision, Writing - review & editing. Xue Jiang: Resources, Writing - review & editing, Funding acquisition, Supervision, Project
Acknowledgements
The authors thank the Foundation of Sichuan Department of Science and Technology (No. 2017FZ0079), Natural Science Foundation of Sichuan Department of Education (No. 17ZB0354) and Foundation of Sichuan Normal University No. 341580001-2016 for financial support. The authors also thank the analytical & testing centre of Sichuan Normal University, and Zhangmei Hu of Southwest Jiaotong University in China for SEM testing.
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