Detection Of Glucose In Human Serum Research Articles

Integrated ratiometric luminescence sensing strategy based on encapsulation of guests in heterobinuclear lanthanide coordination polymer nanoparticles for glucose detection in human serum

Lanthanide coordination polymers (LnCPs) can be used as a host platform to encapsulate functional guest molecules for the construction of integrated sensing platforms. In this work, two guest molecules, rhodamine B (RhB) and glucose oxidase (GOx), were successfully encapsulated in a heterobinuclear lanthanide coordination polymer synthesized by self-assembly of Ce3+, Tb3+ and adenosine monophosphate (AMP) to form RhB&GOx@AMP-Tb/Ce. Both guest molecules show good storage stability and minimal leakage. The higher catalytic activity and stability of RhB&GOx@AMP-Tb/Ce is obtained due to the confinement effect compared to free GOx. RhB&GOx@AMP-Tb/Ce exhibits superior luminescence based on the internal tandem energy transfer process of the nanoparticles (Ce3+→Tb3+→RhB). Glucose can be oxidized in the presence of GOx to form gluconic acid and H2O2. Subsequently, Ce3+ in the AMP-Tb/Ce host structure can be oxidized by H2O2 to Ce4+, thereby interrupt the internal energy transfer process and cause ratiometric luminescence response. Benefiting from the synergistic effect, the smart integrated luminescent glucose probe exhibits a wide linear range (0.4–80 μM) and a low detection limit (74.3 nM) with high sensitivity, selectivity and simplicity, enabling the quantitative detection of glucose in human serum. This work describes a good strategy to construct an integrated luminescence sensor based on lanthanide coordination polymers.

A novel non-enzymatic electrochemical sensor based on NiS/Co3S4@h-Ni NWs core-shell electrode for glucose detection in human serum

To obtain a non-enzymatic electrochemical sensor with good performance such as sensitivity, selectivity, and stability, fine-tuning and rational design of the electrocatalytic material are essential. In this study, a novel catalyst (NiS/Co3S4@h-Ni NWs) with a hierarchical core-shell structure was synthesized in two steps to be used as a non-enzymatic electrode for glucose detection. First, hierarchical nickel nanowires, h-Ni NWs (the core), were prepared by the reduction of Ni2+ ions by hydrazine N2H4, and then the h-Ni NWs are covered with NiS/Co3S4 (the shell) by the hydrothermal method. The resulting NiS/Co3S4@h-Ni NWs showed a core-shell structure with abundant nanotides on the surface and good crystallinity. The prepared sensor exhibited two linearity ranges in the glucose concentration ranges of 0.001–6.57 mM and 6.57–13.32 mM with a sensitivity of 1171.9 μA mM−1 cm−2 and 316.5 μA mM−1.cm−2, respectively, and with a low detection limit of 0.13 μM (S/N = 3) due to its developed core-shell structure that provides excellent conductivity, an efficient mesoporous network, and suitable channels for rapid ion/electron transfer for electrocatalytic activity. In addition, the sensor also showed exceptional selectivity against coexistence interference, good long-term stability, reproducibility, and repeatability. All these excellent results show that the prepared NiS/Co3S4@h-Ni NWs catalyst can be a promising electrode material for glucose detection.

NiCo-LDH nanoflake arrays-supported Au nanoparticles on copper foam as a highly sensitive electrochemical non-enzymatic glucose sensor

The detection of glucose in human blood is of great importance in the diagnosis and prevention of diabetes. In this work, we fabricated a novel electrochemical non-enzymatic glucose sensor, NiCo-LDH nanoflake arrays-supported Au nanoparticles on copper foam (NiCo-LDH@ Au/Cu) by galvanic replacement and electrodeposition methods. Owing to the synergistic effect of three-dimensional (3D) architecture of Cu foam, high electrocatalytic activity of Au nanoparticles and NiCo-LDH nanoflake arrays, the NiCo-LDH@Au/Cu electrode exhibits excellent electrocatalytic ability for glucose oxidation in NaOH solution. Under optimized conditions, the NiCo-LDH@Au/Cu electrode shows excellent activity with a linear range from 0.5 to 3000 μM at the potential of 0.50 V (vs. Ag/AgCl), a low detection limit of 0.23 μM (S/N = 3), an ultra-prompt response time of 0.5 s, and a high sensitivity of 23100 μA mM−1 cm−2, as well as good selectivity and stability. Furthermore, the as-fabricated non-enzymatic glucose sensor was successfully applied to the glucose detection in human serum as a promising candidate in the development of electrochemical non-enzymatic glucose sensor.

Co-Ni layered double hydroxides wrapped on leaf-shaped copper oxide hybrids for non-enzymatic detection of glucose

The leaf-shaped copper oxide (CuO) was first fabricated by a direct precipitation method. Then, the flake-shaped Co-Ni layered double hydroxides (CoNi-LDHs) were grown on the leaf-shaped CuO by using an electrodeposition method to form a unique nanostructured electrocatalyst. Due to the unique structural and compositional advantages, CoNi-LDHs wrapped around the leaf-shaped CuO exhibited good electrocatalytic characteristics. The optimized CuO/CoNi-LDHs exhibited improved non-enzymatic electrochemical sensing performance for glucose, with a reliable linear range (0.1 μM–0.384 mM) and a low limit of detection (0.065 µM, S/N = 3). The utilization of the CuO/CoNi-LDHs sensor for glucose detection in human serum was also corroborated, implying promising potential for glucose monitoring. Results demonstrated that the developed sensor provides new horizons for facile and sensitive glucose detection.

Glucose oxidase decorated fluorescent metal-organic frameworks as biomimetic cascade nanozymes for glucose detection through the inner filter effect.

Metal-organic frameworks (MOFs) as a peroxidase mimic have been integrated with glucose oxidase (GOx) to achieve one-step glucose detection. However, limited by the loading amount of GOx, the performances of the developed glucose sensing assays still remain to be further improved to meet sensing requirements in diverse biological samples. Herein, with Fe3+ as the metal ion and 2-amino-benzenedicarboxylic acid as a ligand, a fluorescent Fe-based organic framework (NH2-MIL-101) with peroxidase-like activity was synthesized. Due to the large specific surface area (791.75 m2 g-1), 68 μg mg-1 GOx could be immobilized through the amidation coupling reaction, and the product was designated GOx@NH2-MIL-101. With OPD as the substrate, Gox@NH2-MIL-101 achieved highly efficient biomimetic cascade catalysis for one-step glucose detection through an inner filter effect: upon reacting with glucose, GOx@NH2-MIL-101 catalytically oxidized glucose using dissolved O2, and the produced H2O2 concurrently oxidized o-phenylenediamine (OPD) to oxidized OPD (oxOPD), accompanied by the fluorescence of GOx@NH2-MIL-101 at 456 nm being quenched and that of oxOPD at 565 nm being enhanced. With the fluorescent ratio F565/F456 used as a readout signal, a wide linear range of 0.1-600 μM was obtained, and the detection limit was 0.0428 μM. Based on the excellent selectivity and high stability of GOx@NH2-MIL-101, the developed assay was successfully applied to glucose detection in human serum and saliva, presenting potential applications in diverse biological samples and even medical diagnosis.

Enhancing the peroxidase activity and decreasing the protease activity of ficin with rational modification and its application to one-step colorimetric detection of glucose.

Ficin has dual enzyme activity, i.e., protease and peroxidase-like activity. In some respects, its application is limited by the protease activity of ficin. Herein, we used tris (2-carboxyethyl) phosphine hydrochloride (TCEP) to break the three pairs of disulfide bonds of ficin, and then blocked the free thiol groups with N-ethylmaleimide (NEM) to synthesize ficin-TN. The results showed that ficin-TN had increased peroxidase-like activity and reduced protease activity. According to this phenomenon, we have exploited a colorimetric method with high sensitivity and selectivity for the one-step detection of glucose. Comparing with ficin, ficin-TN has wider detection range (0.1-300μM) and lower detection limit (88nM), and our method is simpler and more timesaving than other two-step methods. Furthermore, the actual appliances of ficin-TN for glucose detection in human serum have been illustrated with satisfied result, suggesting that its promising utilization in various fields.

Nonenzymatic Glucose Detection in Human Serum Using Ni Nanoparticles Decorated Reduced Graphene Oxide

Reduced Graphene oxide (RGO) decorated with Ni nanoparticles (NiNPs) composites, have been successfully synthesized using a simple hydrothermal method and possessing excellent electrocatalytic activity towards glucose oxidation. The morphological and structural features of RGO-Ni nanocomposites were characterized by field emission scanning electron microscopy (FESEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), Raman spectroscopy, X-ray photoelectron spectroscopy (XPS) and energy dispersive spectroscopy (EDS). From TEM, we observed that NiNPs were anchored on RGO sheets. Cyclic Voltammetric (CV) study revealed that the electrocatalytic activity of RGO-Ni nanocomposite with 20% Ni loading (RGONi-20) towards glucose oxidation is better than that shown by bare Glassy Carbon Electrode (GCE), RGO, bare NiNPs, RGONi10 and RGONi-30. The prepared nanocomposites exhibited fast electrocatalytic response (<5 s) towards glucose oxidation. Amperometric study indicates that the present glucose sensor have exhibited excellent performance by offering a lowest detection limit as 5.1 μM, with linier range from 2 to 5000 μM and high sensitivity of 896.67 μA mM–1 cm–2. Interference from different anticipatable electroactive substances such as ascorbic acid (AA), uric acid (UA) and dopamine (DA) is not observed. Furthermore, the application of the as prepared sensor was successfully demonstrated for the detection of glucose in human serum and results were compa- rable to presently used nonenzymatic technique. RGONi-20 nanocomposite electrode holds great promise for the development of biosensors and other electrochemical devices.

Tungsten disulfide nanosheets-based colorimetric assay for glucose sensing.

We have developed a glucose oxidase (GOx)-mediated strategy for glucose detection, which is based on the intrinsic peroxidase-like activity of WS2 as a catalyst for the 3,3',5,5'-tetramethylbenzidine‑hydrogen peroxide (TMB-H2O2) reaction. The colorimetric assay involves two parts: generation of H2O2 from the oxidation of glucose catalyzed by GOx, and WS2 nanosheets that catalyze the reaction between TMB and H2O2. In this colorimetric assay, the enhancement of colorimetric signals depends directly on the increased H2O2 concentration, which, in turn, relies on the glucose concentration. The results show that the concentrations of the glucose were directly proportional to absorbance of the TMB solutions over a range of 1nM-500μM with a limit of detection of 0.1445nM. In addition, this new colorimetric assay has been utilized for glucose detection in human serum with a satisfactory result.

Synergistic Enhancement Effects of Carbon Quantum Dots and Au Nanoclusters for Cathodic ECL and Non‐enzyme Detections of Glucose

AbstractIn this study, we found that glucose enhance electrochemiluminescence (ECL) intensity of both Au nanoclusters (Au NCs) and carbon quantum dots (CQDs) with K2S2O8 as the co‐reactants. The enhancing effects by Au NCs and CQDs were overlapped, enabling the detection of glucose. The increased ECL intensity of glucose was linear with the logarithm of concentrations of glucose in the range of 50 μM–3.0 mM, and the limit of detection is 20 μM. Anti‐interruption ability was achieved, and ascorbic acid, urea, and uric acid had little influence to glucose detection. This method realized the direct detection of glucose by enhancing ECL of Au NCs and CQDs, which was fast and economic, possessing potential applications for glucose detection in human serum.

Ultra-small and biocompatible platinum nanoclusters with peroxidase-like activity for facile glucose detection in real samples

The highly sensitive glucose detection based on the peroxidase-like properties of nanoclusters has been gained great interest. In this work, Pericarpium Citri Reticulatae polysaccharide (PCRP) stabilized platinum nanoclusters (Pt-PCRP NCs) were prepared by a green method in which potassium tetrachloroplatinate and PCRP were simply mixed without addition of other agents. Platinum nanoclusters (Pt NCs) had ultra-small size of 1.26 ± 0.34 nm. The hydrodynamic size of Pt-PCRP NCs was 29.7 nm, and zeta potential of which was -12.0 mV. Pt-PCRP NCs showed high biocompatibility toward HeLa cells and red blood cells. In addition, Pt-PCRP NCs catalyzed the decomposition of H2O2 to produce •OH, which further oxidized colorless 3,3′5,5′-tetramethylbenzidine (TMB) to blue oxidized 3,3′,5,5′-tetramethylbenzidine (oxTMB), exhibiting peroxidase-like property. The kinetics followed the Michaelis-Menten equation. More importantly, the colorimetric method for glucose detection using Pt-PCRP NCs had high selectivity and low detection limit for 0.38 μM. The established method based on Pt-PCRP NCs was used to precisely detect glucose detection in human serum, saliva, and sweat. Taken together, the prepared ultra-small and biocompatible Pt-PCRP NCs have good potential glucose applications in clinical diagnosis in the future.

Electrochemiluminescent detection of glucose in human serum by BODIPY-based chemodosimeters for hydrogen peroxide using accelerated self-immolation of boronates.

BODIPY-based ECL chemodosimeters were developed for the detection of hydrogen peroxide. The reactivity of boronate towards hydrogen peroxide was enhanced by adjacent fluorine atoms. In combination with glucose oxidase, a fluorine-substituted probe successfully quantified the glucose level in human serum, providing its potential as a versatile tool in point-of-care testing applications.

Well-aligned Cu@C nanocubes for highly efficient nonenzymatic glucose detection in human serum

Unique and well-aligned Cu@C core-shell nanocubes were rationally designed for nonenzymatic glucose detection using cubic Cu2O nanoparticles immerged in water-soluble polyvinyl pyrrolidone (PVP) coatings as precursor. As a consequence, the optimum Cu@C nanocubes with a shell thickness of ∼6.48 nm were prepared by the initial coating of Cu2O nanoparticles with 1.5 mg/mL PVP and subsequent annealing at 600 °C. After thermal annealing process, Cu2O nanoparticles were reduced to Cu nanocubes; at the same time, PVP was pyrolyzed to carbon shell encapulating the cubic Cu core. Due to efficient protection of the carbon shell of Cu core from oxidization and the advantageous inter-connected core-shell conductive networks, the hierarchical Cu@C nanocubes exhibit excellent electrocatalytic activity towards glucose oxidation. Under optimum condition, the resulted 600 °C annealed 1.5 mg/mL-Cu@C/Nafion modified glassy carbon electrode displayed high efficient nonenzymatic glucose detection, offering a wide linear range of 40 μM – 40 mM, with low detection limit at 21.35 μM (S/N = 3) and high sensitivity peak of 2565 μA mM–1 cm–2. More importantly, the well-designed Cu@C core-shell nanocubes could be utilized as a promising nonenzymatic sensor in practical biological applications for the detection of glucose concentration in human serum samples.

A self-activated nanobiocatalytic cascade system based on an enzyme-inorganic hybrid nanoflower for colorimetric and visual detection of glucose in human serum

A new enzyme–inorganic hybrid nanoflower was synthesized and used to achieve a self-activated cascade reaction for glucose detection, and a visual analytical device for screening of the diabetes was also developed. The glucose oxidase–ferrous phosphate hybrid nanoflowers (GOx–Fe3(PO4)2·8H2O HNFs) with two types of morphologies were obtained, in which the nanostructures with hydrangea-like morphology were selected for the subsequent study owing to their excellent catalytic activity. The HNFs exhibited significantly enhanced catalytic activity, stability and reusability compared with free enzymes. In virtue of their good catalytic properties, the HNFs realized the self-activated cascade detection of glucose by integrating two different types of enzymes. First, GOx catalyzed glucose to produce H2O2 and gluconic acid. Then, the generated gluconic acid decreased pH of the reaction system to about 4 which was the optimum pH for Fe3(PO4)2·8H2O to arouse its peroxidase-like activity. The in-situ formed H2O2 was finally catalyzed by adjacent Fe3(PO4)2·8H2O to oxidize 3,3’,5,5’-tetramethylbenzidine (TMB), resulting in a significant color change. This proposed assay has been successfully achieved the glucose detection in human serum with good accuracy and reproducibility. Moreover, a new visual analytical device for screening of the diabetes was developed, which offered a new strategy for the field analysis of glucose.

NiMoO4 nanosheet arrays anchored on carbon cloth as 3D open electrode for enzyme-free glucose sensing with improved electrocatalytic activity.

High electrical conductivity and more active sites exposure are crucial for improving the performance of electrocatalyst. Binary metal oxide nanoarray grown on conductive substrate offers a 3D self-supported electrode with a great promise in boosting its performance in enzyme-free glucose sensing. Here, NiMoO4 nanosheet arrays anchored on carbon cloth (NiMoO4 NSA/CC) was prepared via a simple hydrothermal synthesis and used as 3D self-supported electrode for enzyme-free glucose sensing. The morphology and composition of NiMoO4 nanosheet have been characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), and transmission electron microscopy (TEM). The electrochemical results show that NiMoO4 NSA/CC exhibits remarkable high catalytic activity towards glucose oxidation, with a wide linear response ranging from 1μM to 0.9mM, a high sensitivity of 4.13mA/mM·cm2, and a low detection limit of 1μM (S/N = 3). The enhanced performance might be attributed to the merits of nanosheet arrays with large surface area, self-supported electrode with 3D open network, as well as bimetallic component with high conductivity. Furthermore, NiMoO4 NSA/CC also shows good selectivity and reliability for glucose detection in human serum. This work offers a new pathway for the construction of enzyme-free glucose sensor with high performance. Graphical abstract ᅟ.

Hydrogen peroxide and glucose concentration measurement using optical fiber grating sensors with corrodible plasmonic nanocoatings.

We propose and demonstrate hydrogen peroxide (H2O2) and glucose concentration measurements using a plasmonic optical fiber sensor. The sensor utilizes a tilted fiber Bragg grating (TFBG) written in standard single mode communication fiber. The fiber is over coated with an nm-scale film of silver that supports surface plasmon resonances (SPRs). Such a tilted grating SPR structure provides a high density of narrow spectral resonances (Q-factor about 105) that overlap with the broader absorption band of the surface plasmon waves in the silver film, thereby providing an accurate tool to measure small shifts of the plasmon resonance frequencies. The H2O2 to be detected acts as an oxidant to etch the silver film, which has the effect of gradually decreasing the SPR attenuation. The etching rate of the silver film shows a clear relationship with the H2O2 concentration so that monitoring the progressively increasing attenuation of a selected surface plasmon resonance over a few minutes enables us to measure the H2O2 concentration with a limit of detection of 0.2 μM. Furthermore, the proposed method can be applied to the determination of glucose in human serum for a concentration range from 0 to 12 mM (within the physiological range of 3-8 mM) by monitoring the H2O2 produced by an enzymatic oxidation process. The sensor does not require accurate temperature control because of the inherent temperature insensitivity of TFBG devices referenced to the core mode resonance. A gold mirror coated on the fiber allows the sensor to work in reflection, which will facilitate the integration of the sensor with a hypodermic needle for in vitro measurements. The present study shows that Ag-coated TFBG-SPR can be applied as a promising type of sensing probe for optical detection of H2O2 and glucose detection in human serum.

An iron hydroxyl phosphate microoctahedron catalyst as an efficient peroxidase mimic for sensitive and colorimetric quantification of H2O2 and glucose

An iron hydroxyl phosphate that possesses high peroxidase activity is synthesized via a one-step hydrothermal method and used for colorimetric glucose detection in human serum.

Ni and NiO Nanoparticles Decorated Metal-Organic Framework Nanosheets: Facile Synthesis and High-Performance Nonenzymatic Glucose Detection in Human Serum.

Ni-MOF (metal-organic framework)/Ni/NiO/carbon frame nanocomposite was formed by combing Ni and NiO nanoparticles and a C frame with Ni-MOF using an efficient one-step calcination method. The morphology and structure of Ni-MOF/Ni/NiO/C nanocomposite were characterized by transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), and energy disperse spectroscopy (EDS) mapping. Ni-MOF/Ni/NiO/C nanocomposites were immobilized onto glassy carbon electrodes (GCEs) with Nafion film to construct high-performance nonenzymatic glucose and H2O2 electrochemical sensors. Cyclic voltammetric (CV) study showed Ni-MOF/Ni/NiO/C nanocomposite displayed better electrocatalytic activity toward glucose oxidation as compared to Ni-MOF. Amperometric study indicated the glucose sensor displayed high performance, offering a low detection limit (0.8 μM), a high sensitivity of 367.45 mA M-1 cm-2, and a wide linear range (from 4 to 5664 μM). Importantly, good reproducibility, long-time stability, and excellent selectivity were obtained within the as-fabricated glucose sensor. Furthermore, the constructed high-performance sensor was utilized to monitor the glucose levels in human serum, and satisfactory results were obtained. It demonstrated the Ni-MOF/Ni/NiO/C nanocomposite can be used as a good electrochemical sensing material in practical biological applications.

Ultrasmall Pt Nanoclusters as Robust Peroxidase Mimics for Colorimetric Detection of Glucose in Human Serum.

In this work, a new type of ultrasmall Pt nanoclusters (Pt NCs) was prepared via a facile one-pot approach by using yeast extract as the reductant and stabilizer. Besides their excellent water solubility, these yeast extract-stabilized Pt NCs also possess attractive peroxidase mimicking property. They can efficiently catalyze the oxidation of 3,3,5,5-tetramethylbenzidine (TMB) in the coexistence of hydrogen peroxide (H2O2). Catalytic mechanism analysis suggested that the peroxidase mimicking activity of these Pt NCs might originate from their characteristic of accelerating electron transfer between TMB and H2O2, and their enzymatic kinetics followed typical Michaelis-Menten theory. On the basis of these findings, we developed a new highly sensitive colorimetric method for glucose detection, and the limit of detection was calculated as low as 0.28 μM (S/N = 3). Further application of the present system for glucose detection in human serum has been successfully demonstrated, suggesting its promising utilization as robust peroxidase mimics in the clinical diagnosis, pharmaceutical, and environmental chemistry fields.

Preparation of spinel nickel-cobalt oxide nanowrinkles/reduced graphene oxide hybrid for nonenzymatic glucose detection at physiological level

Nickel-cobalt oxide nanowrinkles with spinel-type crystal structure supported on reduced graphene oxide (NiCo2O4 NWs-rGO) was prepared to develop a sensitive and stable nonenzymatic glucose sensor. The NiCo2O4 NWs-rGO hybrid were prepared by a facile one-pot hydrothermal reaction, and sequential calcination in air. The morphology, composition and crystal structure of the NiCo2O4 NWs-rGO hybrid were characterized by scanning electron microscope, transmission electron microscope, selected area electron diffraction, and energy-dispersive spectroscopy. The electrochemical behavior of the hybrid and its catalytic activity towards glucose oxidation were investigated by several electrochemical methods. Compared with single component NiO or Co3O4, spinel type NiCo2O4 NWs displayed higher catalysis towards glucose oxidation. Further integration of NiCo2O4 with graphene could reduce the overpotential and enhance the catalytic current due to the improved conductivity and dispersity of NiCo2O4. The NiCo2O4 NWs-rGO based glucose sensor showed a wide linear range of 0.005-8.6mM, a low detection limit of 2μM (S/N=3), and an improved stability. A satisfactory recovery was also obtained for glucose detection in human serum at physiological level. Our results indicate rationally combine spinel type mixed metal oxide with graphene is a good alternative to fabricate advanced metal oxide based electrochemical sensors.