Nanoscale Advances
·
2020
·Vol. 2
·期 4
·1583-1589
·
IF 0
Feng Lv,Yuzhu Gong,Yingying Cao,Yaoyao Deng,Shufeng Liang,Xin Tian,Hongwei Gu,Jun-Jie Yin
Effective alcohol detection represents a substantial concern not only in the context of personal and automobile safety but also in clinical settings as alcohol is a contributing factor in a wide range of health complications including various types of liver cirrhoses, strokes, and cardiovascular diseases. Recently, many kinds of nanomaterials with enzyme-like properties have been widely used as biosensors. Herein, we have developed a convenient detection method that combines Au@PtRu nanozymes and alcohol oxidase (AOx). We found that the Au@PtRu nanorods exhibited peroxidase-like catalytic activity that was much higher than the catalytic activities of the Au and Au@Pt nanorods. The Au@PtRu nanorod-catalyzed generation of hydroxyl radicals in the presence of H2O2 was used to develop an alcohol sensor by monitoring the H2O2 formed by the oxidation of alcohol to acetaldehyde in the presence of AOx. When coupled with AOx, alcohol was detected down to 23.8 μM in a buffer solution for biological assays. Notably, alcohol was successfully detected in mouse blood samples with results comparable to that from commercial alcohol meters. These results highlight the potential of the Au@PtRu nanorods with peroxidase-like activity for alcohol detection, which opens up a new avenue for nanozyme development for biomedical applications.
研究领域:
生物传感器
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纳米技术
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分析化学
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生物医学工程
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产品关联
DOI
PubMed
ENVIRONMENTAL POLLUTION
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2024
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IF 7.6
Binrong Li,Chen Wang,Na Li,Chunyang Chen,Zhi Zhu,Xu Tang,Yanhua Cui,Tingting Liu,Collins Kwashie Attatsi,Xuedong Wang
Immobilizing Fe-based nanoparticles on electron-rich biochar has becoming an attractive heterogeneous Fenton-like catalysts (Fe/BC) for wastewater decontamination. However, the insufficient graphitization of biochar causing low electron transfer and by slow H 2 O 2 activation limited its application. Herein, we firstly constructed FeS/biochar composite through all-solid molten salt method (Fe/MSBCs), which can provide strong polarization force and liquid reaction environment to improve carbonization. As expected, the obtained Fe/MSBCs exhibits high surface area and fast interfacial electron transfer between FeS and biochar. More importantly, the partially oxidized FeS (001) facet facilitate H 2 O 2 adsorption and thermodynamically easily decomposition into •OH. Such a synergistic effect endowed them excellent photo-Fenton degradation performance for methyl orange (MO) with large kinetic rate constants (0.079 min −1 ) and high H 2 O 2 utilization efficiency (95.9%). This study first demonstrated the critical regulatory role of molten salt method in iron-based biochar composites, which provide an alternative for H 2 O 2 activator in water pollutant control.
研究领域:
环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
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2024
·
IF 10.7
Jie Yin,Sizhe Li,Hao Zhang,Yao Lu,Yan Zhao,Kai A. I. Zhang
Conjugated polymers (CPs) have garnered attention for their tailorable structure properties, particularly in the context of efficient photosynthetic hydrogen peroxide (H2O2) production. However, the challenge lies in the precise molecular engineering of CPs to facilitate differing reaction pathways, thereby enhancing H2O2 photogeneration efficiency. In this study, we developed dual-chain CPs (DC-CPs) with a distinctive architecture, employing the supramolecular host cucurbit[8]uril as a "molecular lock" to conjoin two polymer chains. The dual-chain configuration is designed to harbour a central reaction centre conducive to oxygen reduction, providing dual conduction pathways for reactant molecules. The existence of this central reaction center was confirmed through the in-situ diffuse reflectance infrared Fourier transform (DRIFT) spectroscopy measurements and density functional theory (DFT) calculations. In addition, femtosecond transient absorption (fs-TAS), variable temperature fluorescence spectroscopy and time-resolved photoluminescence (TRPL) measurements reveal double-stranded structures favourable for carrier transport and reactive site activation between dual polymer chains. Ultimately, DC-CPs demonstrate up to a threefold increase in H₂O₂ production compared to their respective single-chain CPs (SC-CPs). This work adds significantly to the application of CPs for efficient H2O2 photogeneration through molecular engineering strategy.
研究领域:
材料科学
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光催化
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超分子化学
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产品关联
DOI
高影响因子
ACS Nano
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2025
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IF 16
Xiao Ge,Xinya Liu,Jinze Xu,Xiyang Zheng,Li-jiao Tian,Xiaozhi Wang
Rational regulation of the coordination environment of single-atom catalysts (SACs) is a promising yet challenging strategy to enhance their activity. Here, we introduce an O atom into the second coordination shell of Co–N4 sites via a simple thermal treatment, forming a Co–N4–ON matrix to boost photosynthetic hydrogen peroxide (H2O2) production. This modification significantly alters the electronic structure of the Co site, bringing the d-band center closer to the Fermi energy and elevating the conduction band of Co–N4–CN to enhance its reducing capacity. Density functional theory (DFT) calculations reveal intensified charge redistribution and a reduced work function in Co–N4–ON, facilitating O2 adsorption. Notably, Co–N4–ON exhibits the lowest O2 adsorption energy, indicating a stronger interaction between Co–N4–O and O2, which is further strengthened by orbital hybridization and charge transfer at their interface, leading to enhanced O2 activation. The optimized Co–N4–ON catalyst demonstrates superior O2 reduction capabilities with the lowest energy barrier during H2O2 desorption. Consequently, it achieves a H2O2 production rate of 3098.18 μmol g–1 h–1 under neutral conditions, which is 2.6 times higher than that of Co–N4–CN. Moreover, it maintains a production rate of 1967.79 μmol g–1 h–1 over 10 h in a continuous flow reactor under natural sunlight and ambient air, highlighting its durability and practicality. This study underscores the crucial role of the second coordination shell in SACs and offers valuable insights into their atomic-level structure–activity relationships, thus contributing to advancements in catalyst design for efficient photosynthetic H2O2 production.
研究领域:
化学
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材料科学
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环境科学
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产品关联
DOI
PubMed
高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
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2024
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IF 4.4
Xiaojing Song,Libin Yang,Xinyu Chang,Songsong Miao,Hao Zhang
The Na LTA zeolite confined CuO catalyst CuO@Na LTA was prepared via the method of ligand protected in situ with Cu 2+ -glycine complex as Cu source, and characterized by multiple characteristic techniques. The results revealed that CuO nanoparticles were highly dispersed on Na LTA zeolite, and the catalytic properties of CuO@Na LTA were investigated in the alkene epoxidation with H 2 O 2 as oxidant in dioxane. For styrene oxidation, catalyst CuO@Na LTA exhibited excellent catalytic activities with 83 % conversion and 63 % selectivity to styrene epoxide, and could be easily recycled several times without obvious activity loss. The excellent catalytic activities could be attributed to the highly dispersed active CuO species. Besides, multiple electronic effects and coordinative interactions exited in Cu ion and the Si-Al zeolite skeleton framework played a key role in the catalytic recyclability.
研究领域:
化学工程
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材料科学
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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
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2025
·
IF 7.2
Tian Wang,Wei Wang,Yunqing Zhu,Baozhong Zhang
AuNPs/rGO composite cathode was prepared using in-situ reduction method and was applied for H 2 O 2 generation through molecular oxygen (O 2 ) undergoing a 2-electron reduction reaction in the electro-Fenton system. The results showed the AuNPs/rGO cathode exhibited good activity and stability. The size and loading amount of AuNPs, as well as applied voltages were considered for evaluating the catalytic activity of AuNPs/rGO cathode. AuNPs 2:1 /rGO with the smallest size (2.8 ± 0.6 nm) exhibited higher catalytic activity in the electro-Fenton system when the AuNPs 2:1 loading amount was 2.7 %, pH= 3, and applied voltage was −0.6 V (vs. SCE), resulting in an H 2 O 2 yield of 19.3 ± 0.1 mmol g −1 . The synergistic effect of AuNPs 2:1 and rGO enhanced the activation of H 2 O 2 , generating a large number of hydroxyl radicals (∙OH) for efficient degradation of rhodamine B (RhB), corresponding to a degradation efficiency of 100 % within 30 min. In addition, AuNPs 2:1 /rGO exhibited excellent stability and reusability in cyclic experiments. The quenching experiment and the radical spin trap test showed ∙OH and superoxide anion (∙O 2 ̄) as the active species during the reaction process. Furthermore, LC-MS and in-situ FTIR were used to analyze the intermediate products of the degradation process and determine the reaction mechanism.
研究领域:
环境科学
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材料科学
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化学工程
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产品关联
DOI
高影响因子
Journal of Water Process Engineering
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2024
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IF 6.3
Tianmin Gong,Chunmei Gao,Shifeng Ji,Yunqing Xing
2-Methyl-4-chlorophenoxyacetic acid (MCPA) is a herbicide that poses a threat to the environment. In this study, MIL-88A was utilized as a photocatalyst to degrade MCPA. Results demonstrated that the Light/MIL-88A/H 2 O 2 system exhibited remarkable photo-Fenton catalytic activity . Under optimal conditions of pH = 3.8, H 2 O 2 concentration of 1.2 mL/L, MIL-88A dosage of 0.2 g/L and an initial MCPA solution concentration of 50 mg/L, the degradation efficiency reached its peak, achieving a 99.9 % degradation rate of MCPA within 60 min. The morphology, structure, and photocatalytic performance of MIL-88A were investigated using characterization techniques such as SEM, XRD , XPS , and UV–vis DRS . Free radical quenching experiments and ESR characterization demonstrated that the main active material in the degradation of MCPA was •OH. The possible degradation pathways of MCPA were hypothesized by combining the results of Gaussian software and LC-MS analysis. Furthermore, the toxicity of MCPA was evaluated using T.E.S.T. software and mung bean germination experiments. The results revealed that the degradation of MCPA by Light/MIL-88A/H 2 O 2 system could achieve solution detoxification .
研究领域:
环境科学
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化学工程
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产品关联
DOI
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2024
·
IF 5.9
Fuhao Gan,Chunmei Gao,Shifeng Ji,Yunqing Xing,Tianming Gong,Lihui Tian,Yiming Bai,Zhuolong Wu
In this study, the iron-based metal–organic framework MIL-53(Fe) was successfully prepared by a solvent method and used as a photocatalyst for the efficient degradation of DDBAC under visible light. The morphology, structure and photocatalytic properties of MIL-53(Fe) were investigated by SEM, XRD, XPS and UV–vis DRS characterization methods. The optimum conditions for the degradation of DD pathways of DDBAC were analyzed in combination with DFT calculations. Based on molecular orbital theory and free radical quenching experiments, it was demonstrated that hydroxyl radicals were the main contributors in the oxidative degradation of DDBAC. The toxicity of DDBAC and its intermediates was evaluated by culturing Chlorella vulgaris, and the results showed that the Vis/MIL-53(Fe)/H 2 O 2 system was capable of solution detoxification.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
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2025
·
IF 6.5
Yuexia Wang,Jiaqi Xu,Xuan Lin,Chaosi Liu,Xinqing Lu,Yijing Gao,Francesco Pepe,Domenico Caputo,Weidong Zhu
Ti-MWW zeotypes, characterized by their unique dual pore architecture consisting of intralayer 10-membered ring (MR) pore channels and additional interlayer 10-MR pore channels that are interconnected to intracrystalline 12-MR supercages, exhibit a remarkably catalytic superiority in the selective oxidation of small and/or linear alkenes with hydrogen peroxide (H 2 O 2 ), surpassing other titanosilicate zeotypes in performance. However, a further improvement on their catalytic performance is still needed for the industrialization of alkene epoxidation over Ti-MWW. In the present work, the introduction of NH 4 + species into Ti-MWW was conducted via a facile but effective treatment of the as-synthesized zeotypes with NH 4 Cl, named N-Ti-MWW. The comprehensive characterization of N-Ti-MWW, derived from NH 4 + -exchanged Ti-MWW, coupled with Density Functional Theory (DFT) calculations, conclusively demonstrates that the integration of NH 4 + into Ti-MWW promotes the generation of -Ti-OOH hydroperoxo intermediates, resulting in a higher catalytic activity in alkene epoxidation in comparison to the parent one. Moreover, the solvolysis of epoxides is significantly suppressed on N-Ti-MWW, enabling the catalyst to display a superior selectivity towards the targeted epoxide, thereby improving its overall catalytic performance. Additionally, N-Ti-MWW is reusable, after the regeneration of the deactivated catalyst simply treated with NH 4 Cl. As a result, it is anticipated that N-Ti-MWW would be applicable in the industrial epoxidation of alkenes with H 2 O 2 .
研究领域:
化学工程
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材料科学
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产品关联
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2021
·
IF 7.46
Zui Tao,Hewei Si,Xidong Zhang,Jianjun Liao,Shiwei Lin
A highly sensitive and selective sensor is urgently needed in many practical H 2 O 2 detection, such as water quality monitoring, quality control of food products, and so on. However, the traditional three electrode system limits its further development in recent years due to its difficulty in miniaturization and integration. To effectively improve its sensitivity and selectivity, highly-ordered TiO 2 nanotube arrays (TNTAs) are modified with Pt nanoparticles and Prussian blue (PB) nanotubes and creatively combines with thin-film transistor (TFT) based on ZnO to prepare an electrochemical sensor . The sensor uses PBNCs as recognition units for the specific detection of H 2 O 2, and the generated electrical signal is amplified by TFT. Thus, a highly sensitive and selective H 2 O 2 sensor is achieved. The detection limit of the sensor is as low as 5.19 nM, which is three orders of magnitude lower than the conventional electrochemical detection methods using the same electrode. The sensor also possesses wider linear detection range of 0.1–50 μM and 50 μM–5 mM comparable to that of other reported H 2 O 2 sensors. Besides, the sensor has good selectivity for H 2 O 2 in the presence of common interferences such as ascorbic acid , uric acid , glucose, and dopamine. Furthermore, the device presents good reproducibility and exhibits good long-term stability over 27 days of continuous measurement. This study offers important insights for the rational design of sensors with high sensitivity and selectivity.
研究领域:
生物医学工程
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材料科学
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分析化学
✓ 已验证
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Xuefang Zheng,Qi Lian,Liya Zhou,Yanjun Jiang,Jing Gao
A simple and efficient strategy was developed to synthesize polyacrylonitrile-copper oxide (PAN-CuO) nanoflowers by growing copper oxide nanoneedles on the surface of polyacrylonitrile (PAN) nanoflowers under mild conditions. Fortunately, the obtained PAN-CuO nanoflowers exhibit excellent peroxidase-mimicking activity to catalyze the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) to form a blue-colored solution with H2O2. The peroxidase-like mechanism originated from the generation of the •OH radical. The PAN-CuO-based colorimetric assay was used to detect H2O2 with a detection limit (LOD) of 0.12 μM in a linear range from 0.5 to 125 μM. The colorimetric method was simple, selective, and sensitive for ascorbic acid (AA) detection in the range of 1–180 μM with a detection limit (LOD) of 0.56 μM. Moreover, the proposed PAN-CuO-based colorimetric assay could be used in the real sample analysis. The peroxidase-like PAN-CuO nanoflowers could provide a versatile catalytic platform for the application of the colorimetric assay method and biomimetic enzyme catalytic systems, and open a new way for detection of AA in biological systems.
研究领域:
材料科学
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生物化学
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分析化学
✓ 已验证
DOI
高影响因子
CHEMICAL PAPERS
·
2017
·Vol. 72
·期 3
·643-649
·
IF 1.258
Wang Bingtong,Zhang Zongbin,Zhang Xinyu,Sun Shixin,Wu Lin,Xing Rong
A simple, efficient, and eco-friendly catalytic system for the oxidation of cyclohexene to adipic acid with H 2 O 2 catalyzed by H 2 WO 4 in Brønsted acidic ionic liquids under solvent-free conditions has been developed. Reaction conditions such as the catalysts, the types of anions and cations for Brønsted acidic ionic liquids, reaction temperature, and the amount of hydrogen peroxide, were investigated. Moreover, the Hammett acidity functions ( H
0 ) of Brønsted acidic ionic liquids were determined using UV–visible spectrophotometry. The optimum reaction condition identified was n(H 2 WO 4 ):n(Brønsted acidic ionic liquids): n (cyclohexene): n (H 2 O 2 ) = 0.02:0.02:1:4.4, and the yield of adipic acid was 96% under the reaction scale of 10 mmol. The catalytic system can be easily recovered and reused for four reaction runs without significant loss of catalytic activity. Simple operation of the catalyst system and avoidance of the emission of nitrous oxide are the benefits of this work.
研究领域:
化学
·
环境科学
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DOI
高影响因子
危险品化学品经营许可证（带存储）