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SENSORS AND ACTUATORS B-CHEMICAL · 2020 · IF 7.1

A closed bipolar electrochemiluminescence sensing platform based on quantum dots: A practical solution for biochemical analysis and detection

Wenyuan Zhao,Ying Ma,Jianshan Ye,Jiye Jin

Many quantum dots (QDs) are considered as excellent electrochemiluminescence (ECL) fluorophores with high quantum yields (QYs) and good stability. However, their ECL efficiency dramatically decreases in the aqueous solution compared to that in organic phase, which significantly limits their applications in bioanalysis. In this study, we developed a new sensing strategy via the combination of a closed bipolar electrode and electrochemiluminescence (CBP-ECL) system, which allows the separation of sensing in aqueous media and generation of ECL in organic media. Two kinds of QDs, CdSe/ZnS and CsPbBr 3 were applied as ECL fluorophores in this system, and stable, high QYs ECL signals were achieved. The resulting sensing platform demonstrated high sensitivity for the detection of H 2 O 2 with a linear range of 0.02−12 mM and the limit of detection (LOD) of 9.2 × 10 −8 M when CdSe/ZnS QDs were used as ECL reagents. We envision that this system can be widely employed in any kind of bioanalysis which can produce the electrochemical currents in the detecting cell. More importantly, we expect this system could break through the limitation of the fluorophores, especially those with solvent dependent ECL signals such as aggregation-induced emission (AIE) molecules, or most of the hydrophobic dyes.

研究领域: 分析化学 · 生物化学 · 纳米技术 · 电化学
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FOOD CHEMISTRY · 2018 · IF 4.946

Detection of choline and hydrogen peroxide in infant formula milk powder with near infrared upconverting luminescent nanoparticles

Ling Zhang,Shuhan Yin,Jiaze Hou,Wenping Zhang,Hui Huang,Yongxin Li,Cong Yu

Choline is an essential nutrient for the growth and development of the baby, and therefore it is often added to infant formula. In this paper, a novel sensor for choline determination in infant formula is developed based on upconverting nanoparticles (UCNPs) with near infrared luminescence. UCNPs-based detection can avoid the interference of background fluorescence from complex samples, and thus provide high selectivity and sensitivity. It was observed that in the presence of Fe 3+ , polyacrylic acid coated UCNPs were quenched to 3% of its original intensity. The degree of quenching was among the best for UCNPs. Hydrogen peroxide could oxidize Fe 2+ to Fe 3+ , which caused quenching of the upconversion luminescence. A new H 2 O 2 detection method was thus established. In addition, choline could be hydrolyzed to betaine by choline oxidase, and at the same time produced H 2 O 2 , which also caused luminescence quenching through Fe 2+ oxidation. Therefore, selective choline sensing was achieved.

CAS / MDL: 67-48-1
研究领域: 分析化学 · 纳米技术 · 食品科学 · 营养学
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TALANTA · 2018 · IF 4.244

Oriented growth of cross-linked metal-organic framework film on graphene surface for non-enzymatic electrochemical sensor of hydrogen peroxide in disinfectant

Yanli Zhou,Congming Li,Yuanqiang Hao,Baoxian Ye,Maotian Xu

High-density and cross-linked copper-based metal-organic framework (Cu-MOF) sheets were successfully prepared via a simple oriented growth method on a carboxylated graphene-modified electrode surface. Hydrogen peroxide (H 2 O 2 ) was selected as a model molecule to examine the performance of the thin film of Cu-MOF/graphene. The proposed sensor showed an extended linear detection range from 2.00 × 10 −7 to 1.85 × 10 −4 mol L −1 ( R = 0.998), a high sensitivity of 0.792 A (mol L −1 ) −1 , and a low detection limit of 6.7 × 10 −8 mol L −1 , due to the synergistic catalysis from the porous structure and favorable electron transfer mediating function of the electroactive Cu-MOFs and the high conductive property of the graphene. The reduction peak current of H 2 O 2 changed less than 3.7% in the presence of 57-fold high concentrations (2.0 × 10 −4 mol L −1 ) of the potential interfering species. The good selectivity of the prepared modified electrode was acquired by the size exclusion (molecular sieving) for H 2 O 2 because of the proper pore shape and pore size of Cu-MOFs. The feasibility of the assay was verified by test of H 2 O 2 in disinfectant samples. The proposed strategy presents valuable information related to the construction of non-enzymatic electrochemical sensors .

研究领域: 材料科学 · 电化学 · 分析化学 · 传感器
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MOLECULES · 2023 ·Vol. 28 ·期 9 ·3736 · IF 4.6

Platinum Nanoparticles Loaded Graphitic Carbon Nitride Nanosheets with Enhanced Peroxidase-like Activity for H2O2 and Oxidase-Based Sensing

Gege Yang,Ying Chen,Rui Shi,Rongrong Chen,Shanshan Gao,Xin Zhang,Yuan Rao,Ying Lu,Yuancheng Peng,Zhihe Qing,Chunxia Song

Platinum nanoparticles (PtNPs) are classical peroxidase-like nanozyme; self-agglomeration of nanoparticles leads to the undesirable reduction in stability and catalytic activity. Herein, a hybrid peroxidase-like nanocatalyst consisting of PtNPs in situ growing on g–C3N4nanosheets with enhanced peroxidase-mimic catalytic activity ([email protected]–C3N4nanosheets) was prepared for H2O2and oxidase-based colorimetric assay. g–C3N4nanosheets can be used as carriers to solve the problem of poor stability of PtNPs. We observed that the catalytic ability could be maintained for more than 90 days.[email protected]–C3N4nanosheets could quickly catalyze the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB), and the absorbance of blue color oxidized TMB (oxTMB) showed a robust linear relationship with the concentration of H2O2(the detection limit (LOD): 3.33 μM). By utilizing H2O2as a mediator, this strategy can be applied to oxidase-based biomolecules (glucose, organophosphorus, and so on, that generate or consume hydrogen peroxide) sensing. As a proof of concept, a sensitive assay of cholesterol that combined[email protected]–C3N4nanosheets with cholesterol oxidase (ChOx) cascade catalytic reaction was constructed with an LOD of 9.35 μM in a widespread range from 10 to 800 μM (R2= 0.9981). In addition, we also verified its ability to detect cholesterol in fetal bovine serum. These results showed application prospect of[email protected]–C3N4nanosheets-based colorimetry in sensing and clinical medical detection.Keywords:[email protected]–C3N4nanosheets;peroxidase-mimic;H2O2;oxidase-based sensing

研究领域: 纳米技术 · 分析化学 · 生物传感器 · 医学诊断
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INORGANIC CHEMISTRY · 2018 · IF 4.7

MOF-808: A Metal–Organic Framework with Intrinsic Peroxidase-Like Catalytic Activity at Neutral pH for Colorimetric Biosensing

He-Qi Zheng,Chun-Yan Liu,Xue-Yu Zeng,Jin Chen,Jian Lü,Rong-Guang Lin,Rong Cao,Zu-Jin Lin,Jin-Wei Su

Natural enzyme mimetics with high catalytic activity at nearly neutral pH values are highly desired for their applications in biological systems. Herein for the first time a stable MOF, namely MOF-808, has been shown to possess high intrinsic peroxidase-like catalytic activity under acidic, neutral, and alkaline conditions. As a novel peroxidase mimetic, MOF-808 can effectively catalyze the oxidation of 3,3′,5,5′-tetramethylbenzidine when H2O2 serves as oxidant, accompanied by a significant color variation in the solution. The catalytic activity and the color variation were greatly dependent on H2O2 concentration, and thus MOF-808 can be applied to the colorimetric sensing of H2O2. The H2O2 detection limit is 4.5 μM, and the linear range is 10 μM to 15 mM. In view of the significant inhibition effect produced by ascorbic acid, a facile and sensitive approach for colorimetric sensing of ascorbic acid was successfully established. The AA detection limit is 15 μM, and the linear range is 30–1030 μM. Further investigation found that the catalytic activity of MOF-808 could be mainly ascribed to the Zr–OH(OH2) groups. Such active Zr–OH(OH2) groups can be effectively shielded by gluconic acid, and subsequently the catalytic activity of MOF-808 was significantly suppressed. With these findings, a facile and selective colorimetric assay for glucose sensing has been successfully explored via combination of the glucose oxidation with the TMB oxidation. The glucose detection limit is 5.7 μM, and the linear range is 5.7–1700 μM. MOF-808 is one of the best colorimetric biosensors among the peroxidase mimics reported for H2O2, AA, and glucose detection.

CAS / MDL: 9001-37-0
研究领域: 材料科学 · 分析化学 · 生物化学
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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Fluorescent linear polyurea based on toluene diisocyanate: Easy preparation, broad emission and potential applications

Hongyan Cao,Bin Li,Xubao Jiang,Xiaoli Zhu,Xiang Zheng Kong

In contrast to conventional fluorescent polymers featured by large conjugation structures, a new class of fluorescent polymers without above conjugations are gaining constant interest owing to their significant academic importance and promising applications in diverse fields. These unconventional fluorescent polymers are in general composed of heteroatoms (e.g. N, O, P, and S) under different forms. Here we report our recent study on polyurea, prepared by a very simple one step precipitation polymerization of toluene diisocyanate in a binary solvent of water-acetone. This polyurea, basically consisting of phenyl ring and urea group, shows fluorescent emission in a broad concentration range, from very low (10 −5 mg/mL) to its solubility limit (50 mg/mL), and in a wide range of emission wavelength from UV to visible regions of up to 500 nm under varied excitation wavelength. The emission behaviors were fully studied under different concentrations and excitations. It was concluded that the emission in UV region was intrinsic due to the conjugation between the phenyl and the adjacent urea unit; while the emission in visible region, strongly excitation dependent, was caused by the cluster formation of the molecular chains, in accordance with the cluster-triggered-emission (CTE) mechanism. The formation of the cluster was tested through dynamic light scattering, FTIR and UV absorbance. Tested in presence of different metal ions, Fe 3+ demonstrated a quenching effect with high selectivity. Based on this study, different paper-based sensors were designed to detect Fe 3+ , H 2 O 2 in bioanalysis and for data encryption. This work provides a simple way to prepare a polyurea, a novel type of unconventional fluorescent polymer, with high emission performance distinct from its known analogues.

CAS / MDL: 10022-68-1
研究领域: 高分子化学 · 材料科学 · 分析化学 · 生物技术
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY · 2022 · IF 4.831

Rapidly and ultra-sensitive colorimetric detection of H2O2 and glucose based on ferrous-metal organic framework with enhanced peroxidase-mimicking activity

Peipei Huang,Qing Chang,Guodong Jiang,Xu Wang,Haipeng Zhu,Qianqian Liu

In this article, a novel metal–organic framework, namely MIL-101(Fe II ), was firstly synthesized via a facile method. In the presence of H 2 O 2 , MIL-101(Fe II ) possesses excellent peroxidase-like activity toward the classical chromogenic substrate, N, N -Diethyl-p-phenylenediamine sulfate salt (DPD). The substitution of Fe 2+ enhances the construction of Fe(II)-oxo nodes and accelerates electrons transfer between DPD and H 2 O 2 , thereby improving the peroxidase-mimicking catalytic activity of MIL-101(Fe II ) nanoenzyme. Additionally, DPD molecules could be adsorbed readily onto the surface of the nanoparticles due to the π–π interaction. The study of Michaelis constant indicates that the MIL-101(Fe II ) exhibits a higher affinity towards DPD (0.16 mM) in contrast to horseradish peroxidase (0.78 mM). In view of the impressive catalytic performance of MIL-101(Fe II ), two reliable monitoring platforms for the rapid detection of H 2 O 2 and glucose were established with extremely low detection limits of 18.04 nM and 0.87 μM in the ranges of 40–5000 nM and 1.2–300 μM, respectively. The study of the catalytic mechanism indicates that DPD oxidation is attributed to the hydroxyl radical (·OH) produced from the decomposition of H 2 O 2 catalyzed by MIL-101(Fe II ). Furthermore, the developed sensor indicates high selectivity and stability and can be effectively appropriate for the detection of H 2 O 2 and glucose in real samples. This work not only provides a novel nanozyme with superior catalytic performance for biological analysis, but also broadens the application field of MIL-101(Fe II ) material.

CAS / MDL: 6283-63-2 100-21-0
研究领域: 分析化学 · 纳米技术 · 生物催化 · 生物传感器
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ANALYTICAL CHEMISTRY · 2019 · IF 6.35

Fluorescent Graphitic Carbon Nitride-Based Nanozymes with Peroxidase-Like Activities for Ratiometric Biosensing

Xiaoyu Wang,Li Qin,Minjie Lin,Hang Xing,Hui Wei

While breakthroughs in peroxidase-like nanozymes for bioanalysis have been made, most of current nanozyme biosensing systems are based on a single signal output. Such sensing systems could be easily influenced by environmental and personal factors. We envision that nanozyme sensing systems with ratiometric signal outputs would provide more reliable and robust sensing performance. Herein, to construct such ratiometric sensing systems, three fluorescent graphitic carbon nitride (C3N4)-based nanozymes (i.e., C3N4–Ru, C3N4–Cu, and C3N4–hemin) with excellent peroxidase-like activities were prepared. These fluorescent nanozymes emitted a fluorescence at 438 nm when excited at 385 nm. Interestingly, when o-phenylenediamine (OPD) was catalytically oxidized to oxidized OPD (OPDox) in the presence of H2O2 and nanozymes, the OPDox not only emitted an emerging fluorescence at 564 nm but also quenched the fluorescence at 438 nm of the nanozymes. We therefore employed the ratio of the fluorescent intensity at 564 and 438 nm (i.e., F564/F438) as the signal output to construct the ratiometric biosensing systems. First, we used the C3N4–Ru nanozyme to construct the ratiometric H2O2 sensing system, which showed not only the enhanced robustness but also wider linear range and better sensitivity than most reported H2O2 sensors based on nanozymes. Second, with the assistance of glucose oxidase, glucose can be detected by such ratiometric sensing systems. Third, we used three different C3N4-based nanozymes to construct ratiometric sensor arrays for the detection and discrimination of five phosphates. This study provides new insights for constructing robust nanozyme biosensing systems.

研究领域: 生物化学 · 纳米医学 · 分析化学
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MICROCHEMICAL JOURNAL · 2019 · IF 3.206

TMB-assembly as nanosubstrate construction colorimetric kit for highly sensitive and selective detection of H2O2 and monoamine oxidase-A based on Fenton reaction

Can Chen,Shiyu Zhang,Chengwu Zhang,Lin Li,Jixin Zhu,Jinhua Liu

Detection of H 2 O 2 is significant for the applications in environmental protection, pharmaceutical industries , food production, and clinical control. Current colorimetric kit of H 2 O 2 based on enzyme or nanomaterials always needs TMB or other peroxidases substrate as coloration species. Herein, we report a simple hydrothermal method to synthesize of TMB dot as the nanosubstrate construction colorimetric kit for highly selective and sensitive detection of H 2 O 2 based on Fenton reaction . Compared with TMB as the substrate, the synthesized TMB dots (TMBDs) show higher reaction activity in the presence of the same low-level Fe 2+ and H 2 O 2 , resulting in highly sensitive sensing H 2 O 2 down to 0.8 nM. Additionally, the obtained TMBDs can well disperse in solution, while generally TMB as substrate needs to be dissolved in organic solvents such as DMF and DMSO. Furthermore, the developed colorimetric kit is applied in detection of Mao-A, due to the reaction between epinephrine and Mao-A producing H 2 O 2 . More importantly, the proposed method has been successfully applied to the analysis of Mao-A in spiked human serum Hence, the TMBDs as the nanosubstrate provide an efficient, fast and sensitive approach for colorimetric kit of H 2 O 2 and Mao-A, promoting more extensive application in early diagnosis of disease and drug discovery.

研究领域: 分析化学 · 生物化学 · 环境科学 · 药学 · 临床化学
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ANALYTICAL CHEMISTRY · 2016 · IF 5.886

In Vivo Lighted Fluorescence via Fenton Reaction: Approach for Imaging of Hydrogen Peroxide in Living Systems

Changhui Liu,Weiju Chen,Zhihe Qing,Jing Zheng,Yue Xiao,Sheng Yang,Lili Wang,Yinhui Li,Ronghua Yang

By virtue of its high sensitivity and rapidity, Fenton reaction has been demonstrated as a powerful tool for in vitro biochemical analysis; however, in vivo applications of Fenton reaction still remain to be exploited. Herein, we report, for the first time, the design, formation and testing of Fenton reaction for in vivo fluorescence imaging of hydrogen peroxide (H2O2). To realize in vivo fluorescence imaging of H2O2via Fenton reaction, a functional nanosphere, Fc@MSN-FDNA/PTAD, is fabricated from mesoporous silica nanoparticle (MSN), a Fenton reagent of ferrocene (Fc), ROX-labeled DNA (FDNA), and a cationic perylene derivative (PTAD). The ferrocene molecules are locked in the pore entrances of MSN, and exterior of MSN is covalently immobilized with FDNA. As a key part, PTAD acts as not only the gatekeeper of MSN but also the efficient quencher of ROX. H2O2 can permeate into the nanosphere and react with ferrocene to product hydroxyl radical (·OH) via Fenton reaction, which cleaves FDNA to detach ROX from PTAD, thus in turn, lights the ROX fluorescence. Under physiological condition, H2O2 can be determined from 5.0 nM to 1.0 μM with a detection limit of 2.4 nM. Because of the rapid kinetics of Fenton reaction and high specificity for H2O2, the proposed method meets the requirement for real applications. The feasibility of Fc@MSN-FDNA/PTAD for in vivo applications is demonstrated for fluorescence imaging of exogenous and endogenous H2O2 in cells and mice. We expect that this work will not only contribute to the H2O2-releated studies but also open up a new way to exploit in vivo Fenton reaction for biochemical research.

CAS / MDL: 24801-88-5
研究领域: 生物化学 · 纳米技术 · 生物医学工程 · 分析化学
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APPLIED SURFACE SCIENCE · 2023 · IF 6.7

Synergistic effects of Fe-Se dual single-atom sites for boosting electrochemical nonenzymatic H2O2 sensing

Chengcheng Qi,Yuhua Luo,Yongping Dong

The study of single atoms in the field of electrochemical sensing is at the early stage. How to boost the catalytic performance of single atoms is still a big challenge. Herein, we prepare Fe-Se dual single-atom sites on N-doped ultrathin carbon carrier (Fe 1 Se 1 /NC) for realizing highly sensitive nonenzymatic detection of H 2 O 2 . Fe 1 Se 1 /NC was synthesized through the pyrolysis strategy, and then was characterized by transmission electron microscopy (TEM), energy dispersive X-ray spectroscopy (EDS) mapping, high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), X-ray diffraction (XRD), X-ray photoelectron spectrometer (XPS), and electrochemical techniques, respectively. The results displayed that Fe and Se both existed in an atomically dispersed status. Compared to the single-atom Se or Fe catalyst (Se 1 /NC or Fe 1 /NC), the Fe 1 Se 1 /NC significantly boosted the electrocatalytic activity for H 2 O 2 reduction. The Fe 1 Se 1 /NC modified electrode could be used to detect H 2 O 2 in a wide linear range of 0.02 mM to 13 mM with a high sensitivity of 1508.6 µA·mM −1 ·cm −2 and a low detection limit of 11.5 µM. Moreover, the sensor was successfully employed for detecting H 2 O 2 in disinfectant and urine samples. This work provides a novel design of dual-atom catalysts for excellent electrochemical sensing applications.

CAS / MDL: 56-41-7 108-78-1 69-93-2
研究领域: 电化学 · 催化 · 材料科学 · 分析化学
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Journal of Materials Chemistry C · 2022 ·Vol. 10 ·期 18 ·7227-7240 · IF 8.067

Enhancing H2O2 and glucose double detection by surface microstructure regulation of Brussels sprout-like Ni–Co(OH)2/rGO/carbon cloth composites

Xinmeng Zhang,Zixuan Mao,Wanyin Ge,Jiajing Zhu,Yuanxiao Zhao

Surface microstructure regulation is an effective way to enhance the performance of sensing materials. Here, a hierarchical and flexible Brussels sprout-like Ni–Co(OH)2/rGO/carbon cloth (CC) composite was constructed by optimizing the morphology of Ni–Co(OH)2 microspheres and the addition amount of rGO. This sensor shows excellent reproducibility, high selectivity, and good stability. It shows a high sensitivity of 3.7391 mA mM−1 cm−2 in the 0.0388–124.0436 mM line detection range for H2O2 and 1.8457 mA mM−1 cm−2 in the 0.0300–2.0000 mM line detection range for glucose. The low limits of detection for H2O2 and glucose are 2.316 nM and 0.115 μM, respectively. The excellent electrochemical performance of the Ni–Co(OH)2/rGO/CC composite is attributed to its unique Brussels sprout-like microstructure. By studying the electrical conductivity, electrochemical active surface area, and hydrophilic–hydrophobic surfaces of the Ni–Co(OH)2/rGO/CC composite, the structure–performance relationship between the microstructure and sensing performance of the composite was further clarified. Moreover, the mechanism of CC, rGO, and the Ni–Co(OH)2 ternary composite in the sensing process is proposed. This study provides a new strategy for the construction of flexible wearable electrodes with high sensitivity.

CAS / MDL: 7782-42-5
研究领域: 电化学 · 材料科学 · 传感器 · 纳米技术
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