International Journal of Electrochemical Science
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2023
·
IF 1.5
Yuehong Pang,Qiufang Zhang,Xiulan Sun,Jian Ji,Fuwei Pi,Xiaofang Shen
Inspired from the pathogenic process of diphenylalanine (FF) self-assembly, a key structural motif in forming Alzheimer’s β-amyloid peptide fibrils, a facile way for preparation of FF aromatic dipeptide fibrils and fabrication of an electrochemical biosensor were developed. Long persistence length FF fibrils with ultra-high aspect ratio over 1000 were obtained using cationic surfactant assisted evaporation induced self-assembly. The Cotton effects indicate a signature of dominant β-sheet arrangement and the thickness of the β-sheet monolayer is estimated to be 2.38 nm. The obvious blue-shift of intrinsic fluorescence indicates an extended H-aggregate between the phenyl rings in a parallel mode. The FF fibrils based electrochemical biosensor, taking horseradish peroxidase as a model enzyme, displayed an excellent electrocatalytic activity to the reduction of H 2 O 2 . The peak current was a linear function of concentrations ranging from 7.5×10 -7 to 1.4×10 -5 M, with a detection limit of 2.5×10 -7 M. The apparent Michaelis-Menten constant was 7.2 μM. These results indicate that the FF fibrils with ultra-high aspect ratio providing a new and promising platform for construction of electrochemical biosensors.
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Catalysis Science & Technology
·
2023
·Vol. 14
·期 3
·590-597
·
IF 5
Guanglu Xia,Jianhao Qiu,Dingliang Dai,Yong Tang,Zhonghao Wu,Jianfeng Yao
A covalent organic framework (COF) named TpPa-1 was co-modified by chlorine grafting and ZnIn2S4 integration for concurrent photocatalytic H2O2 generation and wastewater purification under visible light. The introduction of electron-withdrawing chlorine groups on TpPa-1 decreases the density of adjacent electron clouds, which promotes the charge carrier separation and the intimate combination with ZnIn2S4 by Cl–Zn/Cl–In bonds, providing an appreciably enhanced photocatalytic activity. Specifically, in pure water, the optimal ZnIn2S4/TpPa-Cl2 sample can achieve a H2O2 yield of 766 μmol L−1, which is 1.5, 2, 7.8 and 5 times those of ZnIn2S4/TpPa-1, TpPa-Cl2, ZnIn2S4 and TpPa-1, respectively. In the tetracycline solution, 95% of tetracycline was degraded and, concomitantly, H2O2 with a yield of 846 μmol L−1 was generated. It is found that H2O2 generation undergoes a two-step O2 reduction with ·O2− as the intermediate, while ·O2−, holes and ·OH are the active species in tetracycline degradation. Likewise, other common pollutants like o-nitrophenol, acid golden yellow and acid red in wastewater could also be effectively degraded along with the appreciable production of H2O2, which realizes the so-called wastewater valorization. This study could advance COF-based photocatalysts and provide a novel insight into wastewater treatment.
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Arabian Journal of Chemistry
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2023
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IF 6
Aijing Li,Xinpeng Chen,Ping Yao,Jun Zhang,Tieling Xing,Guoqiang Chen
In this work, polydopamine (PDA) was used to facilitate the reduction of silver nitrate (AgNO 3 ) to silver nanoparticles (AgNPs) and the simultaneous loading on waste silk fabrics (PDA-SF/AgNPs). The removal activity of the obtained composite PDA-SF/AgNPs on different dyes in the presence of hydrogen peroxide (H 2 O 2 ) and potassium peroxymonosulfate (PMS) was compared. The effects of reaction temperature, H 2 O 2 /PMS dosage, dye concentration, composite dosage, electrolyte concentration and time in two catalyst systems on the dye removal were discussed. The results showed the dye removal of Telon Red A2R reached 81% and 95% in 30–50 min in PDA-SF/AgNPs-H 2 O 2 and PDA-SF/AgNPs-PMS system, respectively. Quenching experiments demonstrated that ·OH, ·O 2 – and SO 4 - · were produced during the degradation process, and the possible degradation pathway of Telon Red A2R were analyzed by HPLC-MS. In addition, the kinetic study indicated that the removal of dye followed quasi-second-order adsorption kinetics. These findings suggest that fabric-based composites have great potential and applications in catalysis and treatment of wastewater.
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ACS Applied Energy Materials
·
2023
·
IF 6.4
Jianghua Yang,Zewen Ji,Shujuan Zhang
The identification of defects and their roles in photocatalytic production of hydrogen peroxide (H2O2) with carbon nitride (CN) is a challenging but important task. Here, a simple route was employed to generate defects in CN by tuning the ratio of the two synthesis precursors: acetylacetone (AcAc) and urea. In this way, a set of modified CNs (AxCN) with dual defects (C doping and surface −OH modification) were successfully fabricated. The one with an AcAc-to-urea ratio (x) of 0.05 showed a photocatalytic H2O2 production rate of 3.6 mmol·g–1·h–1, which was greater than most of the reported CNs. Moreover, the selectivity of H2O2 production was increased from 60% (CN) to 85% (A0.05CN). On the basis of density functional theory and the first-principles calculation, the high performance of A0.05CN was attributed to the synergistic roles of the dual defects in oxygen reduction reactions. The C doping enhanced the anchoring of dioxygen, while the −OH group facilitated the diffusion of charge carriers. The finding here provides an insight into the defect engineering for green generation of H2O2.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
·
IF 9.9
Zhenzhen Guo,Jinwen Zhu,Jian Yin,Peng Miao
In this study, a novel fluorescent biosensor is developed for the detection of H 2 O 2 and glucose based on Zeolitic Imidazolate Framework-8 (ZIF-8) nanocomposites. ZIF-8 encapsulating carbon nanodot (CD) exhibits bright fluorescence emission. After further loading of AgNP, the fluorescence is quenched, which is mainly based on the excited electron transfer from CD to AgNP. Besides, the excitation wavelength of CD falls within the adsorption range of AgNP, which leads to efficient inhibition of the excitation energy. The as-prepared AgNP-CD-ZIF-8 nanocomposites can be utilized as a highly sensitive platform for the analysis of H 2 O 2 and glucose. In the presence of glucose, H 2 O 2 can be generated by the catalysis of glucose oxidase (GOD), which induces the etching of AgNP and subsequent recovery of CD-ZIF-8 fluorescence. This “turn on” biosensor can be applied for facile and convenient quantification of H 2 O 2 . It can also be further extended to detect glucose in real samples after combining specific catalytic effect of GOD. The analytical performances are excellent, which demonstrates great potential for practical utility.
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PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Long Tian,Binyu Zhao,Juan Zhang,Xiaogang Luo,Fengshou Wu
The nanomaterials-based artificial enzymes have attracted great attention because of their high stability, good biocompatibility, high catalytic efficiency, and low cost in recent years. Herein, we synthesized a new covalent organic framework (COFs) through the dehydration reaction of 2,5-dihydroxyterephthalaldehyde and tetra-(4-aminophenyl) porphyrin , which was then used to fabricate the core-shell structured nanospheres (Fe 3 O 4 @COFs) by decorating on magnetic Fe 3 O 4 . In the presence of hydrogen peroxide (H 2 O 2 ), the Fe 3 O 4 @COFs nanospheres were able to catalyze the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) to a blue product (ox-TMB), indicating their high peroxidase-like activity. Based on this phenomenon, the Fe 3 O 4 @COFs was used as a colorimetric probe for sensitive and selective detection of H 2 O 2 and glucose. The detection limit (LOD) of H 2 O 2 was calculated to be 2.6 μM in a linear range from 0.1 to 4 mM, while the LOD of glucose was valued as 6 μM ranging from 0.05 to 0.9 mM. Finally, this method was applied in the determination of the glucose concentration in human serum with high accuracy. Thus, the as-prepared Fe 3 O 4 @COFs could be used as a highly sensitive and selective peroxidase mimic to detect hydrogen peroxide-related molecules, suggesting their great potential in biomedical application.
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Scientific Reports
·
2023
·Vol. 13
·期 1
·1-12
·
IF 4.6
Song Jie,Wan Yating,Yang Chen,Deng Qiuju,Cui Yingde,Yan Zhihong,Liu Yi
In this paper, a novel composite is constructed as a non-enzymatic hydrogen peroxide (H 2 O 2 ) sensor by liquid-phase exfoliation method, which is composed of copper oxide, cuprous oxide and silver nanoparticles doped few-layer-graphene (Cu x O/Ag@FLG). Its surface morphology and composition were characterized by scanning electron microscopy (SEM) and X-ray photo spectroscopy (XPS), and its H 2 O 2 sensing performances include catalytic reduction and quantitative detection were studied with electrochemical methods. Our sensor had a high sensitivity of 174.5 μA mM −1 cm −2 (R 2 = 0.9978) in an extremely wide range of concentrations from 10 μM to 100 mM, a fast response (about 5 s) and a low limit of detection (S/N = 3) of 2.13 μM. The sensor exhibits outstanding selectivity in the presence of various biological interference, such as dopamine, ascorbic acid, uric acid, citric acid, etc. In addition, the constructed sensor continued 95% current responsiveness after 1 month of storage further points to its long-term stability. Last but not least, it has a good recovery rate (90.12–102.00%) in milk sold on the open market, indicating that it has broad application possibilities in the food industry and biological medicine.
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Frontiers in Bioengineering and Biotechnology
·
2023
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IF 5.7
Yujia Liang,Zhengmin Cai,Yamei Tang,Chenglin Su,Liye Xie,Yan Li,Xinqiang Liang
Introduction: Reactive oxygen species (ROS)-mediated therapies have typically been considered as noninvasive tumor treatments owing to their high selectivity and efficiency. However, the harsh tumor microenvironment severely impairs their efficiency. Methods: Herein, the biodegradable Cu-doped zeolitic imidazolate framework-8 (ZIF-8) was synthesized for loading photosensitizer Chlorin e6 (Ce6) and CaO 2 nanoparticles, followed by surface decoration by hyaluronic acid (HA), obtaining HA/CaO 2 -Ce6@Cu-ZIF nano platform. Results and Discussion: Once HA/CaO 2 -Ce6@Cu-ZIF targets tumor sites, the degradation of Ce6 and CaO 2 release from the HA/CaO 2 -Ce6@Cu-ZIF in response to the acid environment, while the Cu 2+ active sites on Cu-ZIF are exposed. The released CaO 2 decompose to generate hydrogen peroxide (H 2 O 2 ) and oxygen (O 2 ), which alleviate the insufficiency of intracellular H 2 O 2 and hypoxia in tumor microenvironment (TME), effectively enhancing the production of hydroxyl radical (•OH) and singlet oxygen ( 1 O 2 ) in Cu 2+ -mediated chemodynamic therapy (CDT) and Ce6-induced photodynamic therapy (PDT), respectively. Importantly, Ca 2+ originating from CaO 2 could further enhance oxidative stress and result in mitochondrial dysfunction induced by Ca 2+ overloading. Conclusion: Thus, the H 2 O 2 /O 2 self-supplying and Ca 2+ overloading ZIF-based nanoplatform for cascade-amplified CDT/PDT synergistic strategy is promising for highly efficient anticancer therapy.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Mingji Xu,Xi Ran,Ruoli Chen,Maoshen Chen,Ruijuan Qi,Chengqin Dai,Chunhua Luo,Hui Peng,Hechun Lin
Gas sensors based on metal/metal oxide heterostructures have shown rapid advancements due to their excellent sensing performance. However, it is difficult to control the formation of Cu/CuO nanostructure due to the easy oxidation of copper and limits its sensing application. Herein, we reported the controlled oxidation of Cu superfine particles (SPs) to form Cu/CuO nanostructure via reducing CuO with monoethanolamine, oxidized with H 2 O 2 and then in-situ annealed at 250 °C. The organic residue generated during the reducing step plays a key role in controlling the oxidation of Cu SPs to form Cu/CuO nanostructure. The nanomaterial was used to fabricate gas sensor, which presents excellent p-type sensing performance to ethanol with good selectivity and a good linear relationship in the range of 1 to 100 ppm ethanol. The response to 100 ppm ethanol can be up to 99.40 under 200 °C operating temperature, and the response under 250 °C is 30.66 with the shorter response and recovery time of 214 s and 74 s, respectively. The sensing mechanism can be explained by the adsorption–desorption model. This study provides a promising strategy for the synthesis of Cu/CuO nanostructure and open a new avenue for the development of highly sensitive ethanol sensor.
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Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 7
·3454-3463
·
IF 11.9
Lei Ding,Jinyan Zhao,Zhikang Bao,Shijie Zhang,Huaijie Shi,Jia Liu,Guoliang Wang,Xiaoge Peng,Xing Zhong,Jianguo Wang
H2O2 and O3 production through electrochemical synthesis is a promising approach to replace anthraquinone processes and corona discharge. However, the simultaneous generation of H2O2 and O3 and the use of their synergistic oxidation to degrade organic contaminants remains a challenge. Herein, heterojunction bifunctional ZnO/ZnS@C electrocatalysts were prepared by a one-step pyrolysis method. ZnO/ZnS@C-750 can achieve 90% selectivity for H2O2 and 11% Faraday efficiency for gaseous O3. The primary contributor to such a performance was exploited to accelerate the electron transfer on the heterogeneous interface and generate more reaction sites. H2O2 and O3 can also be simultaneously generated in the electrolyzer and the synergistic effect of H2O2 and O3 can be utilized to completely degrade organic pollutants, such as phenol and tetracycline. This work provided new insights into the design of the 2e− ORR (oxygen reduction reaction) and EOP (electrochemical ozone production) bifunctional electrocatalysts for pollutant degradation.
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COLLOIDS AND SURFACES B-BIOINTERFACES
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2023
·
IF 5.8
Shuo Liu,Huiqi Yang,Liguo Zhang,Alberto Bianco,Baojin Ma,Shaohua Ge
The injured bone microenvironment is typically characterized by high-level reactive oxygen species (ROS, mainly H 2 O 2 ) and low content of oxygen. The former can cause cell apoptosis, induce immune imbalance and inflammation, inhibit osteogenic differentiation, and delay bone repair . In this work, barrier membranes made of a combination of hydroxyapatite nanowires (HAp NWs) and polylactic acid (PLA) loaded with manganese dioxide nanosheets (NSs) ( [email protected] ) were prepared to guide bone regeneration (GBR). Due to the catalytic function of MnO 2 , [email protected] membranes are able to effectively decompose H 2 O 2 to generate O 2 . In vitro experiments demonstrated [email protected] membranes inhibited the apoptotic process caused by high level of H 2 O 2 , decreased intracellular oxidative stress , suppressed inflammation-related gene/protein expression, and inhibited macrophage M1 polarization. The nanostructured HAp stimulated osteogenic differentiation, and the loading of MnO 2 NSs played a synergistic effect. In addition, the barrier function of PLA could hamper the epithelium overgrowth, providing the development space for periodontal regeneration. By scavenging H 2 O 2 , generating O 2 , eliminating inflammation, and regulating immune response, [email protected] membranes efficiently promoted bone regeneration. Our results confirmed that composite membranes have great potential for application in GBR, and provide a reference for future design of bone repair materials.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Wei Zhou,Liang Xie,Yan Wang,Yani Ding,Xiaoxiao Meng,Fei Sun,Jihui Gao,Guangbo Zhao
Large-scale application of H 2 O 2 production through 2-electron oxygen reduction reaction (2eORR) greatly depends on the cost of electrode materials and configuration. In this work, engineered coal-derived oxygen-rich hierarchical activated coke (AC), which is low-cost and highly tunable in porosity and surface chemistry, was used as catalyst to fabricate gas diffusion electrodes (GDEs) for efficient H 2 O 2 production. Results showed that Fenton’s reagents treatment could significantly increase the contents of C O and –COOH on AC, leading to an increased hydrophilicity. However, the higher O contents do not necessarily enhance the selectivity of AC towards 2eORR (i.e., F-5-AC, F-10-AC), especially that F-20-AC exhibited a complete 4e pathway. GDEs were then fabricated with AC and oxidized AC as catalyst, key fabrication parameters including the PTFE binder and AC particle size, and operating parameters such as current intensity, electrolyte pH, and O 2 flow rate were optimized. Up to 747 mg/L H 2 O 2 were generated within 90 min. Results showed that oxidized AC exhibited a decreased H 2 O 2 yield, due to the flooding of GDEs caused by super-hydrophilicity property. Finally, DFT calculations were employed to reveal the synergistic effect of different O groups considering the fact of high O contents on AC.
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