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ANALYTICA CHIMICA ACTA · 2019 · IF 5.256

Mineralizing gold-silver bimetals into hemin-melamine matrix: A nanocomposite nanozyme for visual colorimetric analysis of H2O2 and glucose

Huan Liu,Yue Hua,Yuanyuan Cai,Luping Feng,Shuai Li,Hua Wang

A nanocomposite nanozyme has been fabricated through mineralizing gold-silver bimetals into Hemin (Hem)-coupled melamine (MA) polymer matrix for visual colorimetric analysis of H 2 O 2 and glucose. Catalytic Hem was cross-linked onto MA scaffold for the mineralization of Au–Ag bimetals yielding the rod-like nanocomposite of MA-Hem/Au–Ag. It was discovered that the resulting nanocomposite could present high aqueous stability and especially improved catalysis, which was more than four-fold higher than that of native Hem. Catalytic kinetics studies indicate that the prepared nanocomposite nanozyme could present much higher affinities to the substrates than those of native Hem or even horseradish peroxidase . Herein, the so mineralized Au–Ag bimetals with the “silver effect” would act as “nanowires” for promoting the electron transferring of nanocomposite nanozyme. Moreover, the Hem-coupled MA polymer matrix with high specific surface area could ensure the high adsorption capacity for the reactant substrates and targeting analytes. The application feasibility of the developed nanocomposite nanozyme was demonstrated subsequently by the colorimetric assays for H 2 O 2 and glucose separately in milk and blood samples, with the linear ranges of 0.010–2.50 mM and 0.0050–2.0 mM, respectively. Such a bimetal mineralization-based fabrication route may open a new door toward the design of diverse nanocomposites nanozymes with improved catalysis and adsorption performances.

研究领域: 材料科学 · 分析化学 · 生物化学
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SOLID STATE SCIENCES · 2021 · IF 3.059

Efficient degradation of tetracycline by H2O2 catalyzed by FeOCl: A wide range of pH values from 3 to 7

Yong Cao,Kangping Cui,Yihan Chen,Minshu Cui,Guanghong Li,Dong Li,Xiaojun Yang

Iron Oxychloride (FeOCl) was prepared by partial thermal decomposition and was studied as a heterogeneous Fenton catalyst to degrade tetracycline (TC). SEM, XRD , XPS technology were used to characterize its performance. The influencing factors of TC degradation efficiency were studied, including pH value, H 2 O 2 content, catalyst dosage and initial TC concentration. The results showed that under the optimal conditions, the degradation rate of 60 mg L −1  TC reached 92.9% within 60 min of reaction. The degradation process follows a second-order kinetic equation. Compared with other iron-based catalysts, FeOCl exhibited better catalytic and degradation effects. Moreover, FeOCl/H 2 O 2 system exhibited a wide pH range (from 3.0 to 7.0) for efficient degradation of TC and showed excellent stability and reusability. Meanwhile, based on the intermediates identified by HPLC-MS, two possible pathways for the degradation of TC were proposed. Further, the results of electron spin-resonance spectroscopy and radical quenching tests suggested that the ·OH formed in the FeOCl/H 2 O 2 system was mainly responsible for the degradation of TC.

CAS / MDL: 3317-61-1 64-75-5
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Materials · 2017 ·Vol. 10 ·期 8 ·868 · IF 2.654

Construction and Characterization of a Chitosan-Immobilized-Enzyme and β-Cyclodextrin-Included-Ferrocene-Based Electrochemical Biosensor for H2O2 Detection

Wenbo Dong,Kaiyin Wang,Yu Chen,Weiping Li,Yanchun Ye,Shaohua Jin

An electrochemical detection biosensor was prepared with the chitosan-immobilized-enzyme (CTS-CAT) and β-cyclodextrin-included-ferrocene (β-CD-FE) complex for the determination of H2O2. Ferrocene (FE) was included in β-cyclodextrin (β-CD) to increase its stability. The structure of the β-CD-FE was characterized. The inclusion amount, inclusion rate, and electrochemical properties of inclusion complexes were determined to optimize the reaction conditions for the inclusion. CTS-CAT was prepared by a step-by-step immobilization method, which overcame the disadvantages of the conventional preparation methods. The immobilization conditions were optimized to obtain the desired enzyme activity. CTS-CAT/β-CD-FE composite electrodes were prepared by compositing the CTS-CAT with the β-CD-FE complex on a glassy carbon electrode and used for the electrochemical detection of H2O2. It was found that the CTS-CAT could produce a strong reduction peak current in response to H2O2and the β-CD-FE could amplify the current signal. The peak current exhibited a linear relationship with the H2O2concentration in the range of 1.0 × 10−7–6.0 × 10−3mol/L. Our work provided a novel method for the construction of electrochemical biosensors with a fast response, good stability, high sensitivity, and a wide linear response range based on the composite of chitosan and cyclodextrin.Keywords:chitosan;catalase;cyclodextrin;ferrocene;composite electrode;electrochemical sensor

CAS / MDL: 9001-05-2
研究领域: 生物化学 · 分析化学
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ANALYST · 2015 ·Vol. 140 ·期 19 ·6684-6691 · IF 4.107

Double enzymatic cascade reactions within FeSe–Pt@SiO2 nanospheres: synthesis and application toward colorimetric biosensing of H2O2 and glucose

Fengmin Qiao,Zhenzhen Wang,Ke Xu,Shiyun Ai

A facile process was developed for the synthesis of FeSe–Pt@SiO2 nanospheres based on the hydrothermal treatment of FeCl3·6H2O, selenium and NaBH4 in ethanolamine solvent, followed by reducing HPtCl4 with NaBH4 in the presence of FeSe particles to obtain FeSe coated with Pt NPs (FeSe–Pt), ending with a surfactant assembled sol–gel process to obtain FeSe–Pt@SiO2. The morphology and composition of FeSe–Pt@SiO2 were characterized by transmission electron microscopy, high resolution TEM, X-ray diffraction and Fourier transform infrared spectroscopy. Structural analyses revealed that FeSe–Pt@SiO2 nanospheres were of regular spherical shape with smooth surfaces due to the SiO2 shells, compared with FeSe particles with 150 nm lateral diameter. The prepared FeSe–Pt@SiO2 nanospheres possessed both intrinsic glucose oxidase (GOx-) and peroxidase-mimic activities, and we engineered an artificial enzymatic cascade system with high activity and stability based on this nanostructure. The good catalytic performance of the composites could be attributed to the synergy between the functions of FeSe particles and Pt NPs. Significantly, the FeSe–Pt@SiO2 nanospheres as robust nanoreactors can catalyze a self-organized cascade reaction, which includes oxidation of glucose by oxygen to yield gluconic acid and H2O2, and then oxidation of 3,3,5,5-tetramethylbenzidine (TMB) by H2O2 to produce a colour change. Colorimetric detection of H2O2 and glucose using the FeSe–Pt@SiO2 nanospheres was conducted with high detection sensitivities, 0.227 nM and 1.136 nM, respectively, demonstrating the feasibility of practical sensing applications. It is therefore believed that our findings in this study could open up the possibility of utilizing FeSe–Pt@SiO2 nanospheres as enzymatic mimics in diagnostic and biotechnology fields.

研究领域: 生物传感 · 纳米医学 · 酶学
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RSC Advances · 2018 ·Vol. 8 ·期 61 ·34877-34882 · IF 2.936

Convenient and sensitive colorimetric detection of melamine in dairy products based on Cu(II)-H2O2-3,3′,5,5′-tetramethylbenzidine system

Xue Han,Zhixin Qin,Mengyao Zhao,Jiajia Song,Fei Qu,Fengli Qu,Rong-Mei Kong

The illegal adulteration of melamine in dairy products for false protein content increase is a strong hazard to human health. Herein, a simple and sensitive colorimetric method was developed for the quantification of melamine in dairy products based on a Cu2+-hydrogen peroxide (H2O2)-3,3′,5,5′-tetramethylbenzidine (TMB) system. In this strategy, Cu2+ exhibits peroxidase-like activity and can catalyze the oxidation of TMB to oxidized TMB (oxTMB) in the presence of H2O2 with a blue colour change of the solution. However, the presence of melamine quickly interacts with H2O2 leading to the consumption of H2O2 and thus strongly hinders the oxidation of TMB. Under the optimal conditions, the absorbance change of oxTMB has a linear response to the concentration of melamine from 1 to 100 μM with a detection limit of 0.5 μM for melamine. The proposed method has many merits including more simplicity, good selectivity, and more cost-effectiveness without using any nanomaterials. The method was further successfully applied to detect melamine in dairy products including milk and infant formula powder.

研究领域: 食品科学 · 分析化学
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RSC Advances · 2016 ·Vol. 6 ·期 23 ·19620-19625 · IF 3.289

Highly sensitive visual detection of catalase based on the accelerating decomposition of H2O2 using Au nanorods as a sensor

Simin Lu,Ling Chen,Ping Yang,Katarzyna Matras-Postolek

The detection of catalase associated with various diseases is very important due to the fact that it is frequently downregulated in human cancer tissues. Noble metal nanomaterial-assisted sensors have achieved rapid development for wide applications but few for detecting catalase. Thus, a novel colourimetric strategy has been developed for the selective and rapid visual detection of catalase by using the decelerating etching of gold nanorods (NRs). In the presence of hexadecyltrimethylammonium bromide and SCN−, which can reduce the redox potential of Au(I)/Au (0), Au NRs would be etched by H2O2 along the longitudinal direction. As a consequence, the colour of solutions changed from bluish green to pink accompanied by the localized surface plasmon resonance (LSPR) extinction peak being shifted to short wavelength. In contrast, the etching process would be prohibited in the presence of catalase, and the colour and LSPR extinction peak of Au NRs would remain unchanged. Furthermore, this Au NR based sensor is applied to test paper that could be used in the detection of catalase in real samples. The discussion of the mechanism indicates that such a sensing method has an ideal performance in terms of sensitivity, selectivity, and linearity.

CAS / MDL: 9001-05-2
研究领域: 生物化学 · 医学诊断 · 纳米技术
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ELECTROCHIMICA ACTA · 2017 · IF 4.798

An enhanced sensitivity towards H2O2 reduction based on a novel Cu metal–organic framework and acetylene black modified electrode

Wei Meng,Shuang Xu,Lei Dai,Yuehua Li,Jing Zhu,Ling Wang

As a large class of highly crystalline hybrid materials, metal-organic frameworks (MOFs) have the potentials to act as electrochemical sensors due to their active metal sites and diverse structures. However, the poor electron-conductive property limits their application as electrocatalyst. An effective strategy is to introduce conductive phases to the MOFs. In this paper, a novel Cu metal–organic framework {[Cu 2 (bep)(ada) 2 ]·H 2 O} n (Cu-MOF) (beb   =   1,4-bis(2-ethylbenzimidazol-1-ylmethyl) benzene, H 2 ada   =   1,3-adamantanediacetic acid) was synthesized under hydrothermal condition. Single-crystal X-ray analysis revealed that the Cu-MOF was a three-dimensional pillar-layered framework with two kinds of paddle-wheel secondary building units. Subsequently, the Cu-MOF modified glassy carbon electrode (GCE) was applied in the H 2 O 2 detection in alkaline solution, and it exhibited the good electrocatalytic activity towards H 2 O 2 reduction. When acetylene black (AB) was added to the Cu-MOF, the electrocatalytic performance of the Cu-MOF modified electrode was greatly improved. The results of amperometric response to H 2 O 2 with different AB addition showed that the Cu-MOF/AB-2%/GCE exhibited a wide linear relationship in the H 2 O 2 concentration range of 0.05–3   μM with a rather high sensitivity of 5.56   μA   μM −1   cm −2 , a low detection limit of 0.014   μM as well as a fast response time of 4   s. The Cu-MOF/AB-2%/GCE also exhibited the good selectivity towards H 2 O 2 reduction, and had no response to its normal co-existences of glucose, glycerin, alcohol and lactose. In addition, the modified electrode showed a good stability in the test period.

研究领域: 化学传感器 · 材料科学 · 电化学
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ELECTROCHIMICA ACTA · 2017 · IF 4.798

Integrated electro-Fenton process enabled by a rotating Fe3O4/gas diffusion cathode for simultaneous generation and activation of H2O2

Yan Zhang,Mingming Gao,Shu-Guang Wang,Weizhi Zhou,Yuanhua Sang,Xin-Hua Wang

In this study, we developed an electro-Fenton (EF) system with a Fe 3 O 4 /gas diffusion electrode (Fe 3 O 4 /GDE) as the rotating cathode, realizing the simultaneous processes of O 2 diffusion, H 2 O 2 generation and activation at the cathode for the first time. In this system, H 2 O 2 was effectively electro-generated on the rotating cathode without external aeration, and then in suit activated to hydroxyl radical by the immobilized Fe 3 O 4 . Experimental results showed that 50   mg   L −1 of tetracycline was completely degraded in 120   min, with the total organic carbon removal efficiency of 56.7%, which was accelerated by 1.7 times compared with the mobilized Fe 3 O 4 as catalyst. This enhancement was ascribed to the increased catalytic ability of immobilized Fe 3 O 4 in the presence of electric field. The effects of some important parameters such as Fe 3 O 4 loading, initial pH, applied potential and the rotation speed were evaluated. Computational fluid dynamics simulation suggested that the rotating disk mode greatly enhanced the mass transfer. Further investigation indicated that the immobilized Fe 3 O 4 contributed to the decomposition of H 2 O 2 predominately, while the effects of leaching iron could be ignored. The hydroxyl radical was considered as the primary reactive oxidants, and the degradation mechanism of tetracycline was proposed combined with the analysis of intermediates by ion chromatograph technology. These findings demonstrated the feasibility of establishing an efficient EF system with a simple and cost-effective integrated cathode based on iron immobilization and rotating GDE for environmental remediation.

CAS / MDL: 9002-84-0 64-75-5
研究领域: 环境科学 · 电化学工程
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Journal of Water Process Engineering · 2025 · IF 6.7

A novel polydopamine-loaded copper sulfide (CuS@PDA) for activating H2O2 to eliminate tetracycline via 1O2 dominated oxidation pathway

Zhou Shi,Chenxi He,Hao Huang,Xile Huang,Tong Hu,Yijia He,Dazhi Yang,Simeng Xia,Haojie Zhang,Lin Deng

The frequently detected antibiotics in aquatic environments can induce antibiotic-resistance genes, thereby posing significant risks to both ecosystems and human health. Thus, it is imperative to remove antibiotics from water environments. We constructed a novel polydopamine-loaded copper sulfide (CuS@PDA) through a simple hydrothermal method to activate H 2 O 2 to degrade tetracycline (TC). Compared to CuS/H 2 O 2 , the CuS@PDA/H 2 O 2 system not only achieved efficient TC removal with kinetic rate constant of 0.20 min −1 , but also showed much lower Cu 2+ ions leaching (3.81 mg/L from CuS vs. 0.21 mg/L from CuS@PDA). Besides, CuS@PDA exhibited remarkable recyclability with 93 % removal in the fifth consecutive cycle. Mechanisms analysis revealed that Cu and S contributed to the H 2 O 2 activation and S promoted the conversion of Cu(II) to Cu(I), beneficial for the production of reactive oxygen species. 1 O 2 was found to play the dominant role in the degradation of TC on the basis of quenching tests and electron paramagnetic resonance (EPR) analysis. PDA in CuS@PDA composites facilitated easier complexation with H 2 O 2 and conferred stronger oxidation capability. Lastly, the TC degradation pathway by CuS@PDA/H 2 O 2 was proposed, and the ecotoxicity of its degradation intermediates was estimated. In conclusion, this work demonstrates that the use of PDA can not only improve the catalytic activity and recyclability of CuS towards H 2 O 2 activation for organic pollutants degradation, but also greatly mitigate copper ions leaching.

CAS / MDL: 10125-13-0 62-31-7
研究领域: 环境科学 · 材料科学 · 生物化学
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Journal of Materials Chemistry A · 2021 ·Vol. 9 ·期 42 ·24056-24063 · IF 12.732

K+, Ni and carbon co-modification promoted two-electron O2 reduction for photocatalytic H2O2 production by crystalline carbon nitride

Yanfang Chen,Xuemei Yan,Jixiang Xu,Lei Wang

H2O2 has a wide range of uses as an oxidant and is also utilized as a high density and environmentally friendly fuel. In this study, crystalline g-C3N4 was modified with K+, Ni and N-doped carbon by thermal-polymerization of Ni2+-anchored and polyvinyl pyrrolidone-encapsulated melamine-cyanuric acid supramolecules, followed by re-calcination in a KCl–LiCl mixture. The obtained strip-like g-C3N4 nanocrystals exhibited high charge separation efficiency and good light absorption capability. Density-functional theory calculations confirmed that the orbital hybridization of Ni–N atoms enabled the formation of charge-transfer channels, which can capture electrons, achieve enhanced oxygen adsorption and reduction via a two-electron pathway. Under the synergistic effects of K+, Ni and N-doped carbon dopants and crystallinity, the obtained sample exhibited high photocatalytic H2O2 yields of 79.6 μM in O2-saturated pure water, which was 10-fold higher than the yield using pristine g-C3N4. This work provides a novel design for production of highly efficient photocatalysts for H2O2 production.

CAS / MDL: 108-78-1 7791-20-0
研究领域: 材料科学 · 环境科学 · 化学
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CHINESE JOURNAL OF CHEMICAL ENGINEERING · 2020 · IF 2.627

Preparation of ZSM-5 containing vanadium and Brønsted acid sites with high promoting of styrene oxidation using 30% H2O2

Xianfeng Liu,Fu Yang,Shuying Gao,Bo Shao,Shijian Zhou,Yan Kong

Design and synthesis of low cost and efficacious industrial catalyst for the oxidation of styrene has been an important research project. Herein, ZSM-5 zeolite containing tetrahedral vanadium (V) and Brønsted acid sites (V-H-ZSM-5) was prepared, and identified by characterizations such as XRD, SEM, UV–vis, NH 3 -TPD, H 2 -TPR N 2 -adsorption/desorption and FTIR. V-H-ZSM-5 performed extremely enhanced catalytic activity for the oxidation of styrene with 30% H 2 O 2 at 40 °C. Moreover, in-situ FTIR spectrum was used to investigate the catalytic mechanism. The results demonstrate that Brønsted acid site could not only increase the adsorption concentration of styrene in the micropores of V-H-ZSM-5 via the π complex interaction between double bond of styrene and Brønsted acid sites, but also increase the oxidation potential of H 2 O 2 . The synergetic action of tetrahedral vanadium (V) and Brønsted acid enhanced the catalytic activity for the oxidation of styrene with 30% H 2 O 2 . Impressively, V-H-ZSM-5 performed high reusability within five runs at a low reaction temperature (40 °C) for the first time.

研究领域: 催化化学 · 材料科学
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES · 2020 ·Vol. 21 ·期 2 ·388 · IF 4.556

Modulation of (Homo)Glutathione Metabolism and H2O2 Accumulation during Soybean Cyst Nematode Infections in Susceptible and Resistant Soybean Cultivars

Xi Chen,Shuang Li,Xuebing Zhao,Xiaofeng Zhu,Yuanyuan Wang,Yuanhu Xuan,Xiaoyu Liu,Haiyan Fan,Lijie Chen,Yuxi Duan

In plant immune responses, reactive oxygen species (ROS) act as signaling molecules that activate defense pathways against pathogens, especially following resistance (R) gene-mediated pathogen recognition. Glutathione (GSH), an antioxidant and redox regulator, participates in the removal of hydrogen peroxide (H2O2). However, the mechanism of GSH-mediated H2O2generation in soybeans (Glycine max(L.) Merr.) that are resistant to the soybean cyst nematode (SCN;Heterodera glycinesIchinohe) remains unclear. To elucidate this underlying relationship, the feeding of race 3 ofH. glycineswith resistant cultivars, Peking and PI88788, was compared with that on a susceptible soybean cultivar, Williams 82. After 5, 10, and 15 days of SCN infection, we quantified γ-glutamylcysteine (γ-EC) and (homo)glutathione ((h)GSH), and a gene expression analysis showed that GSH metabolism in resistant cultivars differed from that in susceptible soybean roots. ROS accumulation was examined both in resistant and susceptible roots upon SCN infection. The time of intense ROS generation was related to the differences of resistance mechanisms in Peking and PI88788. ROS accumulation that was caused by the (h)GSH depletion-arrested nematode development in susceptible Williams 82. These results suggest that (h)GSH metabolism in resistant soybeans plays a key role in the regulation of ROS-generated signals, leading to resistance against nematodes.Keywords:soybean;glutathione;reactive oxygen species;soybean cyst nematode;resistance

研究领域: 植物病理学 · 植物生理学 · 分子生物学
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