ANALYTICAL AND BIOANALYTICAL CHEMISTRY
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2019
·Vol. 412
·期 2
·499-506
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IF 3.286
He Shao-Bin,Chen Feng-Qing,Xiu Ling-Fang,Peng Hua-Ping,Deng Hao-Hua,Liu Ai-Lin,Chen Wei,Hong Guo-Lin
Although a massive research has been devoted on the exploration of noble metal–based nanozyme, less progress has been made in the investigation of palladium (Pd) nanozyme and the interaction between ions and Pd nanozyme. In this study, a new type of Pd nanozyme was prepared by a facile one-pot approach by using carboxylated chitosan as the stabilizer. Owing to the synergistic effect of carboxylated chitosan stabilized Pd nanoparticles (CC-PdNPs) can effectively catalyze the H 2 O 2 -mediated oxidation of 3,3′,5,5′-tetramethylbenzidine sulfate (TMB) accompanied by a blue color change (oxidized TMB), indicating the peroxidase-like activity of CC-PdNPs. Furthermore, the Michaelis-Menten constants and catalytic stability of CC-PdNPs render them suitable for environmental analysis and bio-detection. Here, we found that while introducing the iodine ions (I − ) into the reaction medium, the peroxidase-like activity of CC-PdNPs has been rapidly and effectively inhibited through the formation of Pd-I bond; thus, the active sites of PdNPs can be blocked by I − . Based on this specific inhibition by I − , a facile colorimetric assay has been performed for the detection of I − with an extremely low limit of detection (0.19 nM). Furthermore, the practicality of the proposed sensor also has been demonstrated in tap water, and the satisfactory recoveries were obtained. Our study not only demonstrated a novel Pd–based nanozyme but also provided guidance for I − sensing for environmental analysis, food inspection, and bio-detection.
Graphical abstract
研究领域:
纳米技术
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分析化学
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环境科学
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生物化学
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PubMed
高影响因子
ENVIRONMENTAL POLLUTION
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2024
·
IF 7.6
Jiawen Zhang,Shanjian Liu,Fupeng Huang,Dongmei Bi,Jie Song,Santao Chou
To investigate the impact of different H 2 O 2 concentrations on the Fenton-like systems of H 2 O 2 /biochar, this study examined the mechanism of the physical structure and environmental persistent free radicals (EPFRs) of biochar during diethyl phthalate (DEP) removal by the Fenton-like system. The peak-splitting method was utilized to differentiate EPFRs types in cotton stalk biochar produced at different temperatures. High-temperature environments promote π-electron delocalization, which facilitates phenyl π free radicals and σ-π oxygen-containing free radicals. By analyzing relationships between the removal rate K 1 and removal constant K obs of DEP with the structural properties of biochar, it was discovered that EPFRs concentrations in biochar had a significant positive correlation with K 1 (r = 0.92) and K obs (r = 0.97). Different H 2 O 2 concentrations added to the biochar removal system resulted in varied DEP removal efficiency. Among them, CS 500 , CS 550 , and CS 600 exhibited superior DEP removal efficiency when H 2 O 2 concentration was 5 mM.
研究领域:
环境科学
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化学
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Yanping Cui,Haodong Yang,Xian Xiang,Shibo Zhao,Qiao Huang,Zhaoqiang Huang
A modified graphite felt (MGF) was prepared with carbon black (CB) and polytetrafluoron (PTFE) for cathodic electrochemical H 2 O 2 production, which was used in a flow-through cathodic electro-Fenton reactor to degrade chlorinated hydrocarbons. Cathode electrode was floating on aqueous surface and 369.1 mg/L H 2 O 2 could be produced after 1 h 150 mA power applied without O 2 aeration. The main O 2 source for H 2 O 2 production was confirmed from air with this floating position. In a 2.0 L flow-through cathodic electro-Fenton system, 95.97 % degradation efficiency for 5.0 mg/L trichloroethylene (TCE) was achieved in 90 min with 13.4 mL/min influent rate. Reducing the reactor volume to 0.14 L, 5.0 mg/L TCE could be degraded completely in 10 min with continuous 4 L influent. The mixed chlorinated hydrocarbons (TCE, cis -1,1-dichloroethylene, 1,2-dichloroethane, and dichloromethane) were also rapidly degraded in 20 min. The flow-through cathodic electro-Fenton reactor presented excellent degradation ability for chlorinated hydrocarbons with a smaller volume. In the simulated sand tank system, after continuously operated 27 days, H 2 O 2 concentration in electrode well was still remained at 80 mg/L. In the contaminated field in Tianjin, China, H 2 O 2 yield of MGF in groundwater could keep at about 60 mg/L after 220 min operating.
研究领域:
环境科学
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电化学工程
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Meixuan Wu,Renshu Wang,Lin Miao,Pengfei Sun,Baocheng Zhou,Yubing Xiong,Xiaoping Dong
Pollution of microplastics (MPs) has been drastically threating human health, however, whose elimination from the environment by current approaches is inefficient due to their high molecular weight, strong hydrophobicity and stable covalent bonds. Herein, we report a novel and highly-efficient route to degrade MPs contaminants through synergistically piezocatalytic and Fenton-like activation of H 2 O 2 by a ferroelectric Bi 12 (Bi 0.5 Fe 0.5 )O 19.5 catalyst under ultrasound treatment. For 10 g/L polyethylene terephthalate microplastics (PET-MPs), the synergistic strategy reached a 28.9 % removal rate in 72 h, which is greatly enhanced in comparison to the individual piezocatalysis and Fenton (Fenton-like) activation. By optimizing the types of oxidants (H 2 O 2 , peroxymonosulfate and peroxydisulfate) and bismuth ferrite catalysts (non-piezoelectric Bi 2 Fe 4 O 9 and piezoelectric BiFeO 3 /Bi 12 (Bi 0.5 Fe 0.5 )O 19.5 ), it was revealed that H 2 O 2 is the best oxidant, and the piezoelectric Bi 12 (Bi 0.5 Fe 0.5 )O 19.5 with a high aspect-ratio morphology showed higher activity than the Bi 2 Fe 4 O 9 and BiFeO 3 . The catalyst dosage and H 2 O 2 concentration were further optimized, and the good durability of the catalyst was also demonstrated through multiple uses. Different characterization technologies demonstrated the occurrence of PET-MPs oxidation and fragmentation during the treatment process. The plausible mechanism of synergistically piezocatalytic and Fenton-like H 2 O 2 activation was proposed based on measurements of band structure, piezoelectric property and reactive oxygen species generation. Finally, we detected the intermediates and determined a possible degradation route of PET-MPs. The toxicity assessment indicated that the produced intermediates have low toxicity and potential risks to the environment.
研究领域:
环境科学
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催化化学
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PubMed
高影响因子
ENVIRONMENTAL RESEARCH
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2024
·
IF 7.7
Xuan Luo,Ruiying Zhu,Li Zhao,Xiaobo Gong,Lingrui Zhang,Lu Fan,Yong Liu
Tetracycline hydrochloride (TC) accumulates in large quantities in the water environment, causing a serious threat to human health and ecological environment safety. This research focused on developing cost-effective catalysts with high 2e - selectivity for electro-Fenton (EF) technology, a green pollution treatment method. Defective nitrogen-doped porous carbon (d-NPC) was prepared using the metal-organic framework as the precursor to achieve in-situ H 2 O 2 production and self-decomposition into high activity ·OH for degradation of TC combined with Co 2+ /Co 3+ . The d-NPC produced 172.1 mg L −1 H 2 O 2 within 120 min, and could degrade 96.4% of TC in EF system. The self-doped defects and graphite-nitrogen in d-NPC improved the oxygen reduction performance and increased the H 2 O 2 yield, while pyridine nitrogen could catalyze H 2 O 2 to generate ·OH. The possible pathway of TC degradation was also proposed. In this study, defective carbon materials were prepared by ball milling, which provided a new strategy for efficient in-situ H 2 O 2 production and the degradation of pollutants.
研究领域:
环境科学
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材料科学
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高影响因子
MICROCHEMICAL JOURNAL
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2024
·
IF 4.9
Qi Xiao,Jiawen Li,Shuai Liu,Mingli Yang,Yi Fang,Shan Huang
Given the pivotal role of hydrogen peroxide (H 2 O 2 ) in numerous biological progresses, there has been a recent surge in the development of highly effective electrochemical sensors for H 2 O 2 detection. In this article, we propose an enzyme-free amperometric system for the sensitive and selective recognition of H 2 O 2 , leveraging ultrafine PtPd alloy/ionic liquid-carbon dots (IL-CDs) nanocomposites modified flexible carbon fiber. The IL-CDs were synthesized through the direct electrodeposition of ionic liquid [BMIM][PF 6 ] using Pt sheets as electrodes. Subsequently, a sequential electrodeposition of IL-CDs, H 2 PtCl 6 , and PdCl 2 onto the activated carbon fiber (ACF) yielded the PtPd/IL-CDs/ACF microelectrode. This microelectrode serves as an enzyme-free amperometric sensor for H 2 O 2 detection, exhibiting an improved response with a significantly lower detection limit of 0.29 μM and a relatively broad linear range spanning from 2 to 6561 μM. Furthermore, this enzyme-free amperometric H 2 O 2 sensor demonstrates remarkable stability over extended periods and exceptional performance in practical applications, such as the analysis of commercially available milk, human serum, human urine, and living cancer cells analysis. This study offers a fresh perspective on amperometric sensors based on metal alloys and CDs electrode, highlighting the potential of enzyme-independent detection for hydrogen peroxide in biological systems.
研究领域:
生物医学工程
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分析化学
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Yong Chen,Zhao Yang,Yunbo Liu,Yong Liu
In this paper, a novel Fenton-like system was constructed by a new catalyst (CNTs-Fe-Cu) combined with Al 0 -CNTs to in situ generate H 2 O 2 from activating O 2 for the degradation of sulfamerazine (SMR). The CNTs-Fe-Cu composite was prepared and characterized by XRD, SEM, EDS and BET methods. The results showed that H 2 O 2 could be generated in-situ by Al 0 -CNTs composite under oxygen aeration, which was then converted to OH and O 2 − radical by CNTs-Fe-Cu composite. The high removal efficiency of SMR could be obtained in Al 0 -CNTs/CNTs-Fe-Cu/O 2 system at a relatively broad range of pH. Furthermore, the removal efficiency of SMR and total organic carbon (TOC) was 85% and 60%, respectively under the following condition: initial pH = 5.8, T = 25 °C, O 2 flow rate = 400 mL/min, CNTs-Fe-Cu = 1 g/L, Al 0 -CNTs = 1 g/L, SMR = 50 mg/L, reaction time = 60 min. In addition, the intermediate products of SMR degradation were identified and the possible degradation pathways of SMR and the degradation mechanism of Al 0 -CNTs/CNTs-Fe-Cu/O 2 process were tentatively proposed.
研究领域:
环境科学
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化学工程
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DOI
高影响因子
JOURNAL OF CATALYSIS
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2026
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IF 6
Shiyi Li,Jie Zhang,Bei Liu,Wanchao Hu,Changli Lü
Solar-driven photocatalytic H 2 O 2 production presents a sustainable alternative to the industrial anthraquinone process. An in situ anthraquinone (AQ) functionalized metal–organic framework (UiO-66-F 4 ) with fluorinated linkers enables efficient concurrent synthesis of H 2 O 2 and value-added benzaldehyde (BzH) in a two-phase system. The AQ-modified F-MOF achieves exceptional H 2 O 2 production rates of 118.1mmol g -1 h −1 under visible light and 328.2mmol g -1 h −1 under simulated sunlight, along with high BzH selectivity (∼95%). Fluorinated linkers and AQ act synergistically to enhance the built-in electric field, promote charge separation, and facilitate oxygen adsorption and activation. RDE and RRDE studies verify a highly selective two-electron oxygen reduction pathway (94% H 2 O 2 selectivity) and reveal a non-traditional mechanism involving energy transfer to form electrophilic 1 O 2 , which is subsequently reduced to •O 2 – by electron and protonated to H 2 O 2 . Both experimental and theoretical results demonstrate that the 1 O 2 mediated pathway proceeds with a lower free energy barrier compared to the molecular oxygen route. Meanwhile, the incorporation of AQ reduces the oxygen adsorption energy and provides additional adsorption sites, further enhancing photocatalytic H 2 O 2 production. EPR spectroscopy corroborates the interconversion between 1 O 2 and •O 2 – during the reaction. This work offers mechanistic insight into the coexistence and interconversion of reactive oxygen species, while demonstrating spontaneous separation and collection of both H 2 O 2 and high-value oxidation products in a two-phase system.
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高影响因子
JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2026
·
IF 9.2
Yidan Liu,Lejing Zhou,Li Zhao,Dianrui Yang,Xiaobo Gong,Yong Liu
A novel nitrogen-doped porous carbon catalyst (NCW) was synthesized via in-situ growth of ZIF-8 on balsa sawdust followed by controlled carbonization. The integration of ZIF-8 significantly increased specific surface area, defect density, and electrochemical activity, while nitrogen incorporation—especially pyridinic and graphitic species—enhanced 2e − oxygen reduction reaction (ORR) selectivity, achieving an exceptional H 2 O 2 selectivity of 94%. When immobilized on a graphite cathode and paired with a boron-doped diamond (BDD) anode, the NCW-based electro-Fenton (EF) system enabled robust in-situ H 2 O 2 generation and efficient tetracycline (TC) degradation. Under optimized conditions, the system achieved a maximum H 2 O 2 accumulation of 0.73 mmol L −1 , completed TC removal within 120 min, and a total organic carbon (TOC) mineralization efficiency of 84.6% after 4 h. Quenching experiments and electron paramagnetic resonance (EPR) spectroscopy identified homogeneous and heterogeneous hydroxyl radicals (·OH) and superoxide radicals ( ‐ O 2 · ‐ ) as the key reactive species. The NCW/BDD/EF system demonstrated excellent versatility across various organic pollutants and maintains robust reusability over multiple cycles. This work presents a sustainable strategy for developing wood-derived electro-Fenton catalysts for efficient antibiotic wastewater treatment.
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高影响因子
BIOELECTROCHEMISTRY
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2026
·
IF 4.9
Zijie Pi,Yuanyuan Zhang,Rongqin Yang,Lin Liu,Yu Huang,Yingchi Wu,Tao Gou,Honghao Kang,Tao Zhang,Xiaoling Yang,Xiaoling Liao
A high-performance nanozyme electrochemical sensor was engineered for the sensitive detection of hydrogen peroxide (H 2 O 2 ). The sensor is based on a synergistic ternary nanocomposite of ZIF-8, reduced graphene oxide (RGO), and platinum nanoparticles (Pt NPs). In this design, the Pt NPs serve as the catalytic centers with intrinsic peroxidase-like activity, effectively mimicking natural enzymes to catalyze the electrochemical reduction of H 2 O 2 . This nanocomposite was immobilized on a glassy carbon electrode (GCE) via a combined drop-casting and electrodeposition strategy. Morphological and structural analyses using scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDS), and X-ray photoelectron spectroscopy (XPS) confirmed the successful fabrication of a uniform nanocomposite architecture. Systematic optimization revealed that the sensor exhibited excellent detection performance for H 2 O 2 , with a sensitivity of 22.3 μA mM −1 cm −2 ( n = 4), a detection limit as low as 59 nM (S/N = 3), a limit of quantification of 0.197 μM, and a linear range of 62 nM–13.07 mM, exhibiting good selectivity and reproducibility. Importantly, the sensor was successfully applied for the real-time, in-situ monitoring of H 2 O 2 released from zebrafish embryos under cadmium ion (Cd 2+ ) induced oxidative stress. This work offers a promising tool for the early assessment of heavy metal-induced oxidative damage.
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高影响因子
Journal of Water Process Engineering
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2025
·
IF 6.7
Di Wu,Huilin Huang,Aiping Zhang
Although copper-based Fenton-like processes can remove refractory organics from the membrane bioreactor effluent of landfill leachate (referred to as MBR effluent), the kinetic limitations of the Cu 2+ /Cu + cycling lead to oxidant consumption, which further restricts the degradation efficiency. To address this issue, the microwave (MW)/CuS/H 2 O 2 Fenton-like process (pH = 3.0, MW = 160 W, CuS = 96 mg/L, [H 2 O 2 ] = 75 mM, t = 15 min) was used to treat the MBR effluent. The results showed that this process efficiently removed UV 254 (69.26 %) and color number (CN, 94.45 %) and significantly reduced the degree of polymerization, aromaticity, and molecular weight of organics in the MBR effluent. Further reactive species experiments confirmed the presence of hydroxyl radicals ( • OH), singlet oxygen ( 1 O 2 ), and superoxide radicals (O 2 •− ) in the process, with O 2 •− acting as the primary reactive species. On the basis of the changes in the CuS morphology and valence state, it was indicated that the main mechanism of the MW/CuS/H 2 O 2 Fenton-like reaction is a synergy between homogeneous and heterogeneous Fenton-like processes, and the thermal effect of MW accelerated the cycling of the Cu 2+ /Cu + and the generation of reactive species. Finally, after 6 cycles of the CuS catalyst, the removal efficiency of benzoic acid (BA) remained above 70 %. This confirms the structural and chemical stability of CuS. This study provides a reference for overcoming the kinetic limitations of copper-based Fenton-like processes and improving the removal efficiency of refractory organics from the MBR effluent.
研究领域:
环境科学
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化学工程
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高级氧化技术
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废水处理
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污染控制
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高影响因子
MICROCHIMICA ACTA
·
2025
·Vol. 192
·期 7
·1-12
·
IF 5.3
Xu Zixuan,Zhang Yumin,Jiang Minqiang,Wang Yuheng,Li Min,Li Lijie,He Gaohong,Zhang Wenjun
Of tunable porosity, high specific surface area and excellent stability, the metal–organic frameworks (MOFs) as nanozyme capably not only catalyze the bio-substrate but load the natural enzyme, so as for the cascade catalyzation achievement. However, the limited mass transfer rate and natural enzyme abscission of MOFs are still fatal for the practical application. Herein, taking P-aminobenzoic acid (PABA) as a pore-size regulator and boronic acid (BA) as the bio-affinity sorbent, BA-MIL-100(Fe)-PABA of enlarged pores and better affinity was acquired as the peroxidase to ensure the efficient mass transfer and enzyme protection. Via the thorough investigation, the maximum reaction rate of H 2 O 2 catalyzation by BA-MIL-100(Fe)-PABA was up to 2.62 × 10 −7 M·s −1 with \({K}_{m}\) as low as 0.357 mM, along with the LOD of 0.77 μM. Loading GOx, a cascade platform of GOx@BA-MIL-100(Fe)-PABA was subsequently obtained to detect the blood glucose stable-selectively, with the wide linear response range (0.025–1.5 mM) and the LOD of 0.017 mM. The recycled catalytic activity of the platform was better 68% during 12 cycles. A new method for constructing defective MOFs at room temperature was thus proposed to achieve an efficient mass transfer and a better bio-affinity for glucose detection with high sensitivity and selectivity, paving the way for more sensitive detection and advanced applications. Graphical abstract
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高影响因子
危险品化学品经营许可证（带存储）