High-performance Glucose Sensor Research Articles

Controlled synthesized of ternary Cu-Co-Ni-S sulfides nanoporous network structure on carbon fiber paper: a superior catalytic electrode for highly-sensitive glucose sensing

BackgroundEfficient monitoring of glucose concentration in the human body necessitates the utilization of electrochemically active sensing materials in nonenzymatic glucose sensors. However, prevailing limitations such as intricate fabrication processes, lower sensitivity, and instability impede their practical application. Herein, ternary Cu-Co-Ni-S sulfides nanoporous network structure was synthesized on carbon fiber paper (CP) by an ultrafast, facile, and controllable technique through on-step cyclic voltammetry, serving as a superior self-supporting catalytic electrode for the high-performance glucose sensor.ResultsThe direct growth of free-standing Cu-Co-Ni-S on the interconnected three-dimensional (3D) network of CP boosted the active site of the composites, improved ion diffusion kinetics, and significantly promoted the electron transfer rate. The multiple oxidation states and synergistic effects among Co, Ni, Cu, and S further promoted glucose electrooxidation. The well-architected Cu-Co-Ni-S/CP presented exceptional electrocatalytic properties for glucose with satisfied linearity of a broad range from 0.3 to 16,000 μM and high sensitivity of 6829 μA mM− 1 cm− 2. Furthermore, the novel sensor demonstrated excellent selectivity and storage stability, which could successfully evaluate the glucose levels in human serum. Notably, the novel Cu-Co-Ni-S/CP showed favorable biocompatibility, proving its potential for in vivo glucose monitoring.ConclusionThe proposed 3D hierarchical morphology self-supported electrode sensor, which demonstrates appealing analysis behavior for glucose electrooxidation, holds great promise for the next generation of high-performance glucose sensors.

An origami microfluidic paper device based on core-shell Cu@Cu2S@N-doped carbon hollow nanocubes

BackgroudThe global prevalence of diabetes mellitus, a serious chronic disease with fatal consequences for millions annually, is of utmost concern. The development of efficient and simple devices for monitoring glucose levels is of utmost significance in managing diabetes. The advancement of nanotechnology has resulted in the indispensable utilization of advanced nanomaterials in high-performance glucose sensors. Modulating the morphology and intricate composition of transition metals represents a viable approach to exploit their structure/function correlation, thereby achieving optimal electrocatalytic performance of the synthesized catalysts. ResultsHerein, a sensitive and rapid Cu-encapsulated Cu2S@nitrogen-doped carbon (Cu@Cu2S@N–C) hollow nanocubes-functionalized microfluidic paper-based analytical device (μ-PAD) was fabricated. Through a delicate sacrificial template/interface technique and thermal decomposition, inter-connected hollow networks were formed to boost the active sites, and the carbon shell was coated to protect Cu from being oxidation. For application, the constructed μ-PAD is used for glucose sensing utilizing an origami automated sample pretreatment system enabled by a simple application of strong alkaline solution on wax paper. Under optimal circumstances, the Cu@Cu2S@N–C electrochemical biosensor exhibits broad detection range of 2–7500 μM (R2 = 0.996) with low detection limit of 0.16 μM (S/N = 3) and high sensitivity of 1996 μA mM−1 cm−2. Additionally, the constructed μ-PAD also exhibited excellent selectivity, stability, and reproducibility. SignificanceBy rationally designing the double-shell hollow nanostructure and introducing Cu-encapsulated inner layer, the synthesized Cu@Cu2S@N–C hollow nanocubes show large specific surface area, short diffusion channels, and high stability. The proposed origami μ-PAD has been successfully applied to serum samples without any additional sample preparation steps for glucose determination, offering a new perspective for early nonenzymatic glucose diagnosis.

Smartphone based wearable sweat glucose sensing device correlated with machine learning for real-time diabetes screening

BackgroundDiabetes is a significant health threat, with its prevalence and burden increasing worldwide indicating its challenge for global healthcare management. To decrease the disease severity, the diabetic patients are recommended to regularly check their blood glucose levels. The conventional finger-pricking test possesses some drawbacks, including painfulness and infection risk. Nowadays, smartphone has become a part of our lives offering an important benefit in self-health monitoring. Thus, non-invasive wearable sweat glucose sensor connected with a smartphone readout is of interest for real-time glucose detection. ResultsWearable sweat glucose sensing device is fabricated for self-monitoring of diabetes. This device is designed as a body strap consisting of a sensing strip and a portable potentiostat connected with a smartphone readout via Bluetooth. The sensing strip is modified by carbon nanotubes (CNTs)-cellulose nanofibers (CNFs), followed by electrodeposition of Prussian blue. To preserve the activity of glucose oxidase (GOx) immobilized on the modified sensing strip, chitosan is coated on the top layer of the electrode strip. Herein, machine learning is implemented to correlate between the electrochemical results and the nanomaterial content along with deposition cycle of prussian blue, which provide the highest current response signal. The optimized regression models provide an insight, establishing a robust framework for design of high-performance glucose sensor. SignificanceThis wearable glucose sensing device connected with a smartphone readout offers a user-friendly platform for real-time sweat glucose monitoring. This device provides a linear range of 0.1–1.5 mM with a detection limit of 0.1 mM that is sufficient enough for distinguishing between normal and diabetes patient with a cut-off level of 0.3 mM. This platform might be an alternative tool for improving health management for diabetes patients.

Copper-based bimetallic metal–organic framework in-situ embedded of heterogeneous Cu nanoparticles for enhanced nonenzymatic glucose sensing

Copper-based metal–organic frameworks (MOFs) are recently emerging as encouraging electrocatalysts with high performance and stability for electrochemical detection of glucose. Herein, a simple one-step solvothermal in-situ derivative strategy is proposed to fabricate the novel heterogeneous electrocatalyst of Cu nanoparticles embedded bimetallic Cu@MCu-BDC-NH2 (M = Ni, Co and Zn) MOFs, which can enhance the conductivity via tailor the electronic structure and heterojunction interface. The optimal bimetallic Cu@CoCu-BDC-NH2 heterostructure exposes more active sites, the electronic interaction between metal-O enhanced the reactivity and electrical conductivity, and prominently boost the kinetics of glucose detection. The optimized Cu@CoCu-BDC-NH2 heterojunction structure as modified electrode nanomaterials exhibit the low detection limit (0.27 μM), wide linear range (0.5 μM–2 mM) and the high sensitivity (21157 μA mM−1 cm−2), which are successfully used in human serum and hold great stability and anti-interference. The density functional theory (DFT) calculation demonstrates that the adsorption energies of Cu@CoCu-BDC-NH2 heterostructure for glucose are −0.3 eV, suggesting good adsorption capacity for glucose. This work not only successfully establish Cu nanoparticles heterostructure interface with bimetallic MOFs for high-performance glucose sensors, but also emphasizes the importance of regulate the electronic microstructure of bimetallic MOFs for enhanced reaction kinetics.

Tunable Non-Enzymatic Glucose Electrochemical Sensing Based on the Ni/Co Bimetallic MOFs.

Constructing high-performance glucose sensors is of great significance for the prevention and diagnosis of diabetes, and the key is to develop new sensitive materials. In this paper, a series of Ni2Co1-L MOFs (L = H2BPDC: 4,4'-biphenyldicarboxylic acid; H2NDC: 2,6-naphthalenedicarboxylic acid; H2BDC: 1,4-benzenedicarboxylic acid) were synthesized by a room temperature stirring method. The effects of metal centers and ligands on the structure, compositions, electrochemical properties of the obtained Ni2Co1-L MOFs were characterized, indicating the successful preparation of layered MOFs with different sizes, stacking degrees, electrochemical active areas, numbers of exposed active sites, and glucose catalytic activity. Among them, Ni2Co1-BDC exhibits a relatively thin and homogeneous plate-like morphology, and the Ni2Co1-BDC modified glassy carbon electrode (Ni2Co1-BDC/GCE) has the highest electrochemical performance. Furthermore, the mechanism of the enhanced glucose oxidation signal was investigated. It was shown that glucose has a higher electron transfer capacity and a larger apparent catalytic rate constant on the Ni2Co1-BDC/GCE surface. Therefore, tunable non-enzymatic glucose electrochemical sensing was carried out by regulating the metal centers and ligands. As a result, a high-sensitivity enzyme-free glucose sensing platform was successfully constructed based on the Ni2Co1-BDC/GCE, which has a wide linear range of 0.5-2899.5 μM, a low detection limit of 0.29 μM (S/N = 3), and a high sensitivity of 3925.3 μA mM-1 cm-2. Much more importantly, it was also successfully applied to the determination of glucose in human serum with satisfactory results, demonstrating its potential for glucose detection in real samples.

A 1 mm ×1 mm CGM System on Die Achieving 1.65-nA/mM In Vivo Resolution and 0–40-mM/L Detection Range With ΔΣ Backscatter Technique

Diabetes has become a leading cause of death and disability all over the world. Continuous glucose monitoring (CGM) based on wireless power transfer (WPT) and backscatter communication enables wireless real-time telemetry to control glycemic levels in a long term. However, conventional backscatter techniques in CGM systems converted the sensing current into a bit stream or a frequency signal to switch the antenna, leading to two drawbacks: 1) Large power-harvesting antennas are required to complement the power loss in data converting and antenna switching and 2) Both the resolution and detection range are limited even with a high-performance glucose sensor. In this work, we propose a <inline-formula xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink"> <tex-math notation="LaTeX">$\Delta\Sigma$</tex-math> </inline-formula> backscatter technique to demonstrate a system on die (SoD) within a 1 <inline-formula xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink"> <tex-math notation="LaTeX">$\times$</tex-math> </inline-formula> 1-mm on-chip antenna. Implemented in the 65-nm CMOS process, the proposed SoD achieves a telemetry error less than 0.25% with little impact on WPT, as well as a wide detection range of 0–40 mM/L. In vivo experimental results show that the CGM SoD realizes a resolution of 1.65 nA/mM.

In situ growth of the CoO nanoneedle array on a 3D nickel foam toward a high-performance glucose sensor.

A glucose sensor with high sensitivity and low detection limit is vital for human beings' health. Herein, a CoO nanoneedle array with an unique electronic structure was successfully constructed by a hydrothermal and subsequent high-temperature calcination process. The optimized CoO-400 nanoneedles exhibit a larger electrochemical active surface area, beneficial electronic structure, favorable lattice distortion, and abundant active sites, which effectively promote electrochemical properties toward glucose sensing. The glucose sensor constructed by CoO-400 nanoneedles shows a high sensitivity of 84.23 mA cm-2 mM-1 and low detection limit of 4.4 × 10-7 M, superior to the results from most previous reports. Moreover, outstanding anti-interference ability, superior long-term stability, good repeatability, and satisfactory reproducibility in glucose detection for CoO-400 nanoneedles are also demonstrated.

Novel Ni-Co-S Nanospheres Decorated Zralconi-O Nanotube Amorphous Electrodes as High-Performance Glucose Sensors

Novel Ni-Co-S Nanospheres Decorated Zralconi-O Nanotube Amorphous Electrodes as High-Performance Glucose Sensors

Bifunctional Ag@Ni-MOF for high performance supercapacitor and glucose sensor

In this work, Ag nanoparticles (NPs) doped Ni-MOF was prepared by hydrothermal synthesis followed by chemical reduction. The size of Ag NPs is about 20 nm and dispersed between the nanosheets of Ni-MOF, which increases the surface area and pore size of Ni-MOF. As a result, the specific capacitance of the Ag@Ni-MOF electrode increases from 820 F/g (Ni-MOF) to 1312 F/g at a current density of 1 A/g due to the improved conductivity and enhanced diffusion of electrolyte. After 3000 cycles of charge-discharge, the remaining specific capacitance is 80% of the initial value in a two-electrode system, compared with the low cycle stability of Ni-MOF (60%). Moreover, the Ag@Ni-MOF coated GCE electrode displays excellent electrochemical performance as a non-enzymatic glucose sensor. In 0.1 M NaOH solution and under 0.5 V working voltage, the composite electrode exhibits a wide linear detection range of 5–500 μM and a sensitivity of 160.08 μA cm−2 mM−1. The detection limit reaches 5 μM (S/N = 3). Meanwhile, the Ag@Ni-MOF/GCE electrode reveals good performance in the anti-interference experiment and stability experiment as well.

Construction of highly accessible single Co site catalyst for glucose detection

The development of high-performance glucose sensors is an urgent need, especially for diabetes mellitus diagnosis. However, the glucose monitoring is conventionally operated in an invasive finger-prick manner and their noninvasive alternatives largely suffered from the relatively poor sensitivity, selectivity, and stability, resulted from the lack of robust and efficient catalysts. In this paper, we design a concave shaped nitrogen-doped carbon framework embellished with single Co site catalyst (Co SSC) by selectively controlling the etching rate on different facet of carbon substrate, which is beneficial to the diffusion and contact of analyte. The Co SSC prompts a significant improvement in the sensitivity of the solution-gated graphene transistor (SGGT) devices, with three orders of magnitude better than those of SGGT devices without catalysts. Our findings expand the field of single site catalyst in the application of biosensors, diabetes diagnostics and personalized health-care monitoring.

Highly sensitive non-enzymatic wireless glucose sensor based on Ni–Co oxide nanoneedle-anchored polymer dots

Polymer dot (PD)-bridged nickel cobalt oxide (NiCo2O4 (NCO)) nanoneedle-assembled globe-shaped clusters for high-performance glucose sensors were prepared via the consecutive calcination and packaging of PDs using the hydrothermal technique. The sp2-conjugated bridge of electrons, abundantly available catechol functionalized active sites offered by the PDs, and porous structure of NCO created effective electron transport routes for electrocatalytic reactions. The remarkable synergy between the conductive PDs and NCO conferred the PDs-bridged NCO (PDs-NCO) exceptional electrocatalytic activity for glucose detection. Under the optimal applied potential of +0.5 V, the developed PDs-NCO-coated Ni foam (NF) electrode presented the broad detection range from 5 μM to 0.25 mM, sensitivity of 806.17 μA mM−1 cm−2, detection limit of 2.75 μM, and exceptional selectivity. Furthermore, the PDs-NCO-coated NF electrode achieved the specific capacitance of 35.63 F g−1 at the current density of 0.5 A g−1 and superb cycling stability including the 96.7% specific capacitance retention over 5000 charge-discharge cycles. In addition, glucose-sensing could be easily monitored using a wireless sensor on a smartphone. The combination of NCO and PDs represents an innovative approach for constructing high-performance, reusable, non-enzymatic glucose sensors with low detection limit, high sensitivity, and excellent selectivity.

NiMoO4 nanoparticles decorated carbon nanofiber membranes for the flexible and high performance glucose sensors

The free-standing and flexible carbonaceous nanofiber membrane (CNF) comprising of NiMoO4 nanoparticles decorated carbon fibers were developed for glucose sensing analysis. The applicability of polymeric nanofiber membranes in electrochemical sensors is accelerated by enhancing their electrical conductivity via carbonization process. The cavities exist in CNFs accelerate the rapid diffusion of glucose and maximizes the analyte utilization efficiency. The uniform implantation of catalytic active sites of NiMoO4 on CNFs accelerates the glucose sensing kinetics further. With the synergism of bimetal active sites, porous architecture, and conductive carbon network, NiMoO4/CNF demonstrates the excellent sensitivity, low detection limit, and broad linear range, respectively, of 301.77 μA mM−1 cm−2, 50 nM, and 0.0003–4.5 mM toward glucose sensing. Also, the sensing concerts of NiMoO4/CNF are reliable, repeatable, and electrochemically stable along with the high specificity and real sample applicability toward glucose detection. Thus, the free-standing, bendable, binder-free, reusable, and cost-efficient fabrication process developed for the NiMoO4/CNF membrane realizes it’s conscription in the development of cost-efficient and high performance glucose sensors.

Ultrathin CuxO nanoflakes anchored Cu2O nanoarray for high-performance non-enzymatic glucose sensor

Designing highly active material to fabricate high-performance glucose sensor was great importance for diabetes treatment. In this work, we develop a novel nanocomposite composed of multilevel nanostructure with ultrathin CuxO nanoflakes anchored on Cu2O nanowires, directly on Cu foil and its application as non-enzymatic glucose sensor. Due to more active sites endowed by the ultrathin CuxO nanoflakes, the as-prepared CuxO nanoflakes/Cu2O nanowires@Cu nanoarray exhibit high sensitivity (3.59 mA mM−1 cm−2), low detection limit (0.69 μM), high selectivity, fast amperometric response (~ 2 s) and excellent reliability in human serum. And the sensitivity of ultrathin CuxO nanoflakes/Cu2O nanowires@Cu nanoarray was 1.9-fold than that of Cu2O nanowires@Cu nanoarray. Such novel multilevel nanoarray synthesized by convenient method provides a facile way to design metal oxide nanomaterial for promising non-enzymatic glucose sensor.

Transfer-free CVD graphene for highly sensitive glucose sensors

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.

Metal/metal oxide@carbon composites derived from bimetallic Cu/Ni-based MOF and their electrocatalytic performance for glucose sensing

A metal/metal oxide@carbon composite(M/MO@C) was prepared by the direct carbonization of bimetallic Cu/Ni-based MOF (Cu/Ni-MOF) to make M/MO nanoparticles distributed well over the porous carbon matrix. The results of XRD and XPS corroborated the existence of Cu2O, CuO, Ni and NiO in M/MO nanoparticles. Due to a synergistic advantage from Cu2O/CuO, Ni/NiO and porous carbon, M/MO@C-800 exhibited an excellent sensing performance to glucose with a wider linear range from 0.1μM to 2.2mM and a lower detection limit of 0.06μM. Moreover, M/MO@C-800 also possessed an impressive reproducibility, excellent stability and high selectivity. The satisfactory detection of the glucose in the real samples demonstrated that M/MO@C had a perspective application as a high-performance glucose sensor.

One-step microwave-assisted synthesis and characterization of novel CuO nanodisks for non-enzymatic glucose sensing

In this study, a new approach for glucose sensing emphasizing on cost-effectivity and simplicity while sensitivity of sensor remains high enough, is proposed. In this respect, we prepared CuO nanodisks having an ellipsoidal form without using any template or surfactants just by using microwave irradiation for 5min and used it to modify disposable commercial screen printed carbon electrodes(SPCE) without using any kind of binders like nafion. The synthesized CuO nanostructure has been thoroughly characterized using various complementary techniques (SEM, TEM, FT-IR, XRD) while the performance of proposed electrochemical sensor was investigated as for glucose sensing. Different effective parameters on performance of the electrochemical sensor, including KOH concentration, applied potential, repeatability, stability and selectivity, were investigated and discussed. The linear dynamic range, from 2.0μM to 2.5mM, with detection limit of 0.2μM (at signal to noise ratio of 3) and sensitivity of 627.3μAmM−1cm−2, are comparable or better than many of more sophisticated glucose sensors. Therefore, this simple and sensitive sensor can offer a cost-effective and high-performance glucose sensor with respect to previously reported copper oxide based glucose sensors. Capability of proposed sensor for measurement of glucose was evaluated in human urine sample.

A Renewable Platform for High-Performance Glucose Sensor Based on Co(OH)2 Nanoparticles/Three-Dimensional Graphene Frameworks

Co(OH)2 nano particles (NPs)/three-dimensional graphene frameworks (3DGFs) nano-materials was fabricated via electrochemical methods. The Co(OH)2 NPs/3DGFs hybrid retain the 3DGFs's structure and have superior catalytic activity for glucose oxidation. The electrochemical sensors based on Co(OH)2 NPs/3DGFs exhibited high sensitivity of 2410 μA cm−2mM−1, wide linear range of 2 μM to 1.4 mM, low detection limits of 0.67 μM and a quick response (less than 3s) to glucose. The Co(OH)2 NPs/3DGFs were used as a high performance platform to detect glucose in human serum, fetal bovine serum, and human urine. The excellent catalytic activity of Co(OH)2 NPs/3DGFs is attributed to the high surface area of 3DGFs and the highly catalytic activity of Co(OH)2 NPs as well as the synergistic effects between Co(OH)2 NPs and 3DGFs. Importantly, the electrochemical glucose sensor could be renewable only being refreshed in 0.1 M NaOH for ten minutes.

Graphene/nano-ZnO hybrid materials modify Ni-foam for high-performance electrochemical glucose sensors

The detection of glucose has been attracting more and more attention. The present work provided a novel glucose sensor based on graphene/zinc oxide nanoparticle nanocomposite modified Ni foam to fabricate an electrode (G-ZnO/Ni foam). The structure and morphology of the electrode were characterized by SEM, XPS, and XRD. And the electrochemical performance of G-ZnO/Ni foam electrode was evaluated using cyclic voltammetry (CV) and amperometry analysis. The resulting electrode exhibited excellent electrocatalytic activity toward the reduction of glucose in a linear range of 50–1000 μmol with a correlation coefficient of 0.986. The sensitivity of the graphene/zinc oxide nanocomposite modified Ni foam sensor was 1635.52 μA mM−1 cm−2. It is has better electrochemical performance for glucose and is promising in high-sensitivity detection of glucose applications.

MOF-derived in situ growth of carbon nanotubes entangled Ni/NiO porous polyhedrons for high performance glucose sensor

The carbon nanotubes entangled Ni/NiO porous polyhedrons were obtained by in situ growing process with Ni-MOF precursor acting as both the carbon source and catalyst (Ni/NiO) source, which showed highly improved electrochemical performance. The enhanced glucose oxidation activity of Ni/NiO/CNTs may be due to the synergistic effect of metallic nickel and carbon nanotubes.

3D CuO nanosheet wrapped nanofilm grown on Cu foil for high-performance non-enzymatic glucose biosensor electrode

3D binder-free CuO nanosheets wrapped nanofilms has been in situ synthesized on Cu substrate by a simple and facile procedure, with an aim of fabricating high-performance glucose sensor. The complex morphology that the nanosheet grown on Cu subtract evolved into nanofilms and eventually converged to nanowires, is benefit for the mass transport and electro-catalysis. Compared the ECSA of the CuO modified electrode to that of the bare Cu electrode, the effective surface area during the electro-catalysis of the CuO/Cu electrode is much larger. The glucose sensor based on CuO products exhibited high sensitivity (4201μAcm−2mM−1), low detection limit (0.5μmol/L) and quick response time (0.7s). And the stability and selectivity is also fantastic. According to the serum sample analysis, it transpires that the CuO/Cu sensor displayed excellent recovery compared to the concentration values measured by medial method. So this material shows great potential applications in glucose sensors.