Journal of Environmental Sciences
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2022
·
IF 6.796
Jie Xu,Yang Guo,Qian Yang,Xueling Bai,Runhua Lu,Menghui Liu,Zichen Kuang,Luo Zhang,Jing Li
Ultraviolet/persulfate (UV/PS) and Ultraviolet/hydrogen peroxide (UV/H 2 O 2 ) have attracted much attention in recent years as advanced oxidation processes for water treatment. However, it is not all clear how these two methods affect the formation of cyanogen chloride (CNCl) in the subsequent water chlorination process. In this study, it was found that both UV/H 2 O 2 and UV/PS pre-oxidation promoted the formation of CNCl in six actual water samples collected from urban rivers. Glycine, uric acid, arginine and histidine were investigated as the model compounds to explore the effects of different methods on the production of CNCl. The results showed that compared with chlorination alone, pre-oxidation by UV/H 2 O 2 and UV/PS can reduce the production of CNCl for glycine and uric acid by up to 95% during post-chlorination process. However, they can greatly promote the formation of CNCl for arginine and histidine by up to 120-fold. In a more detailed investigation, pre-oxidation of histidine formed highly reactive intermediates to chlorine, leading to increased CNCl formation and chlorine consumption. The results showed that the precursors of CNCl was altered after pre-oxidation, and need to be re-evaluated.
研究领域:
环境科学
·
水污染控制工程
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PubMed
高影响因子
ANALYTICA CHIMICA ACTA
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2021
·
IF 6.558
Kuan-Neng Chi,Yan Guan,Xi Zhang,Tong Yang,Shuang Meng,Rong Hu,Yun-Hui Yang
The analytical methods based on colorimetric detection of various analytes have attracted intensive interest. However, most of them display relatively low sensitivity. Herein, a novel colorimetric strategy based on iodide/metal-organic frameworks (MOF)-mediated amplification was developed for low-cost, naked-eye detection and quantification of H 2 O 2 ,Cr 2 O 7 2− , and H 2 S. Cu-MOFs could catalyze the oxidation of the colorless peroxidase substrate TMB to produce a blue product. The published researches mainly focused on the immobilization or integration of a macromolecule , such as natural enzymes , to enhance MOFs catalytic abilities. The use of small molecules to improve the catalytic performance of MOFs has rarely reported. Due to the negligible steric hindrance , iodide could easily be adsorbed in the framework pore of MOFs to conduct the synergic catalytic effect, and shows a high catalytic effect. As a result, the catalytic activity of Cu-MOFs was dramatically enhanced, and thus, the nanocatalyst could act as an amplifier system for target detection. The detection limits obtained by the amplified method are 25, 30, and 0.2 nM, respectively, which are about 200-fold lower than that of the unamplified colorimetric assays . The colorimetric strategy developed herein provides a novel system for the detection of low concentrations of analytes in complex biological samples.
研究领域:
分析化学
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生物医学
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PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Feijian Xiao,Dezhi Yang,Chun Xun,Haiyan Li,Qiulan Li,Zitao Zhong,Daqiao Wei,Yaling Yang
Nanozymes have drawn increasing attention due to unique enzyme-mimic catalytic activities for the treatment of bacterial infections. Herein, a novel tri-metal nanozyme for synergistic eradication of Escherichia coli ( E. coli ) and Staphylococcus aureus ( S. aureus ) was generated by Mo/Fe doped carbon dots (Mo/Fe-CDs) wrapping copper peroxide (CuO 2 ) nanozyme (Mo/Fe@CuO 2 ). Mo/Fe@CuO 2 showed near-infrared (NIR) light-enhanced peroxidase-like catalytic activity, and H 2 O 2 self-supply to promote the generation of reactive oxygen species (ROS) for highly efficient antibacterial photothermal therapy. The CuO 2 could generate H 2 O 2 in the acidic microenvironment, and Mo/Fe-CDs consequently could convert H 2 O 2 to hydroxyl radicals (·OH), resulting in the improvement of sterilization efficiency. Interestingly, Mo/Fe-CDs could activate the transformation of Cu 2+ to Cu + through the co-catalytic reaction based on the Mo 4+ /Mo 6+ and Fe 3+ /Fe 2+ redox couples, and provided photonic hyperthermia (PTT) to enhance the peroxidase-like activity. Meanwhile, Mo/Fe@CuO 2 showed glutathione (GSH) oxidase-like activity, which can achieve the depletion of glutathione (GSH) in bacteria, thus significantly improving the bactericidal effect. The collaborative eradication of bacteria, through innovative metal carbon-based nanozyme technology, provides a powerful and feasible approach to treating bacterial infections that threaten human health.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Pan Xia,Lele Zhao,Xi Chen,Zhihong Ye,Zhihong Zheng,Qiang He,Ignasi Sirés
On-site H 2 O 2 electrosynthesis via two-electron oxygen reduction reaction (ORR) is attracting great interest for water treatment. The use of carbon black-based gas-diffusion electrodes (GDEs) is especially appealing, but their activity, selectivity and long-term stability must be improved. Here, a facile GDEs modification strategy using trace polymethylhydrosiloxane (PMHS) allowed reaching a outstanding H 2 O 2 production, outperforming the conventional polytetrafluoroethylene (PTFE)-GDE (1874.8 vs 1087.4 mg L −1 at 360 min). The superhydrophobicity conferred by PMHS endowed the catalytic layer with high faradaic efficiencies (76.2%−89.7%) during long-term operation for 60 h. The electrochemical tests confirmed the high activity and selectivity of the PMHS-modified GDE. Moreover, the efficient degradation of several micropollutants by the electro-Fenton process demonstrated the great potential of the new GDE. An in-depth understanding of the roles of PMHS functional groups is provided from DFT calculations: the −CH 3 groups contribute to form a superhydrophobic interface, whereas Si-H and as-formed Si-O-C sites modulate the coordination environment of active carbon centers.
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高影响因子
MICROCHEMICAL JOURNAL
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2023
·
IF 4.8
Yijing Ai,Fan Shi,Xiao Han,Xiaoqing Li,Wanting Fu,Baoli Wang,Xiaoping Zhang,Wei Sun
In this work, a simple one-step pyrolysis process was designed to synthesize Fe-doped graphite carbon nitride (Fe–C 3 N 4 ) nanosheets with FeCl 3 as Fe source. The resulted samples were characterized by various characterization techniques, and the results showed that Fe species might form Fe–N bonds with N atoms of C 3 N 4 , which was similar to the iron (Ⅲ) porphyrin active center of horseradish peroxidase. Then Fe–C 3 N 4 nanosheet was further mixed with carbon nanotube (CNT) to obtain Fe–C 3 N 4 @CNT nanocomposite, which was further modified on the self-made flexible printed electrode (PE) to construct the flexible working electrode. Fe–C 3 N 4 nanosheets show good catalytic activity for H 2 O 2 and the introduction of CNT can effectively improve the electron transfer efficiency at the modified electrode interface. By combining with wireless portable electrochemical workstation, the sensor shows a wider detection range (10.0 μmol/L–20.0 mmol/L) and a lower limit of detection (0.38 μmol/L, S/N = 3) for the H 2 O 2 analysis. Furthermore, the sensor can be applied to the real time and in-situ analysis of H 2 O 2 secreted from live cells. In word, this self-supported sensing electrode shows great potential applications in monitoring the pathological and physiological dynamics of cancer cells.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
·
IF 9.028
Jingjing Hu,Sen Wang,Jiaqi Yu,Wenkai Nie,Jie Sun,Shaobin Wang
Heterogeneous electro-Fenton (HEF) reaction has been considered as a promising process for real effluent treatments. However, the design of effective catalysts for simultaneous H2O2 generation and activation to achieve bifunctional catalysis for O2 toward •OH production remains a challenge. Herein, a core–shell structural Fe-based catalyst (FeNC@C), with Fe3C and FeN nanoparticles encapsulated by porous graphitic layers, was synthesized and employed in a HEF system. The FeNC@C catalyst presented a significant performance in degradation of various chlorophenols at various conditions with an extremely low level of leached iron. Electron spin resonance and radical scavenging revealed that •OH was the key reactive species and FeIV would play a role at neutral conditions. Experimental and density function theory calculation revealed the dominated role of Fe3C in H2O2 generation and the positive effect of FeNx sites on H2O2 activation to form •OH. Meanwhile, FeNC@C was proved to be less pH dependence, high stability, and well-recycled materials for practical application in wastewater purification.
研究领域:
环境科学
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材料科学
·
催化化学
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DOI
PubMed
高影响因子
ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2021
·Vol. 413
·期 8
·2135-2146
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IF 4.157
Mei He,Ma Yange,Wu Huimin,Wang Xuedong
Herein, we synthesized and characterized glutathione-capped copper nanoclusters (CuNCs) using a convenient one-pot chemical reduction approach based on glutathione as capping and reducing agents. The Ce(III) induced aggregation-induced emission of CuNCs to form a CuNCs-Ce 3+ fluoroprobe due to electrostatic and coordination interactions between Ce 3+ and CuNCs. In contrast to CuNCs, the fluorescent intensities (FLs) of CuNCs-Ce 3+ were enhanced by ~ 40-fold concomitant with 20-nm blue-shift of the maximum emission, and a 3.45-fold lengthening of the average fluorescent lifetime. The FLs of CuNCs-Ce 3+ were selectively quenched at 650 nm by hydrogen peroxide (H 2 O 2 ) via the redox reaction. Based on this phenomenon, the sensitive assay of H 2 O 2 was realized, and the linear range spanned over the range of 14–140 μM. Notably, the visualization of the fluorescence quenched effect of H 2 O 2 could be easily attained. Additionally, glucose could be specifically oxidized by glucose oxidase to produce H 2 O 2 , and thus the detection of glucose was achieved according to changes in the concentrations of H 2 O 2 . Under optimized conditions, the fluorescent assay of glucose based on the CuNCs-Ce 3+ system offered the linear range of 8–48 μM with detection limit of 2.4 μM. Meanwhile, high selectivity of the as-constructed fluorescent assay allows the sensitive detection of H 2 O 2 and glucose in real-world care products and human serum samples, showing a great application potential in their conventional monitoring.
研究领域:
分析化学
·
生物医学
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DOI
PubMed
高影响因子
Journal of Nanomaterials
·
2020
·
IF 1.98
Qiong-Qiong Ren,Fen Yang,Wu Ren,Chang Wang,Wen-Shuai Jiang,Zong-Ya Zhao,Jun Chen,Xuan-Yi Lu,Yi Yu
An enzyme-based amperometric biosensor was fabricated for detecting hydrogen peroxide (H2O2). Horseradish peroxidase (HRP) was modified using functionalized fluorescent gold nanoclusters (AuNCs) via biomineralization. HRP-AuNCs were successfully immobilized on multiwalled carbon nanotube- (MWCNT-) coated carbon fiber ultramicroelectrodes (CFUMEs). The AuNCs, which act as molecular electric wires, effectively promote the electron transfer between the enzyme active center and the electrode. Additionally, the HRP conjugated with the AuNCs retains its biological activity, which enables the catalytic reaction of H2O2. The HRP-AuNCs/MWCNTs/CFUMEs have been proven as excellent amperometric sensors for H2O2. The sensitivity of the H2O2 biosensor is , and the detection limit is estimated to be 443 nM. Furthermore, the biosensor exhibited long-term stability and good reproducibility. Moreover, the biosensor has been tested by determining the H2O2 concentration in calf serum samples.
研究领域:
生物化学
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纳米技术
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分析化学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2020
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IF 5.774
Weike Zhao,Bo Zhou
In recent years, multi-walled carbon nanotubes (CNTs), which are emerging nanocatalysts, have received much attention in advanced oxidation processes. CNTs were introduced into H 2 O 2 /Fe(III) Fenton-like process to enhance the degradation of bisphenol A (BPA) in this study. The results of the study suggests that CNTs could effectively promote electron transfer from H 2 O 2 to Fe(III) and directly reduce Fe(III) to Fe(II) to accelerate Fe(III)/Fe(II) cycles, in which carbonyl groups and structural defects of CNTs were identified as the major active sites via SEM, Raman, XRD, FTIR and XPS analyses. It was revealed that hydroxyl radical (·OH) majorly contributed to the degradation of BPA, and the generation efficiency of ·OH was significantly increased by 3.2 times with the addition of CNTs. Also, nine intermediate products were identified, and the possible degradation pathways of BPA were proposed through the density functional theory (DFT) calculations and HPLC-MS/MS analysis. The ecotoxicity evaluation of BPA demonstrates that the oxidative degradation of BPA in CNTs/H 2 O 2 /Fe(III) system could effectively reduce its environmental risk. The critical experimental parameters including the dosage of Fe(III), H 2 O 2 , CNTs, initial pH and various anions (Cl − , HCO 3 – , SO 4 2− ) were investigated, and the reusability experiments indicate that CNTs maintained high stability and reusability during the reaction.
研究领域:
环境科学
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化学工程
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高影响因子
Analytical Methods
·
2014
·Vol. 6
·期 19
·7973-7977
·
IF 1.938
Yingfeng Qin,Liangliang Zhang,Gaojie Ye,Shulin Zhao
A homogeneous label-free colorimetric sensing strategy for bleomycin (BLM) assay was developed on the basis of BLM enhanced Fe(II)–H2O2–ABTS reaction. Fe(II) exhibits a catalytic effect on H2O2-mediated oxidation of ABTS by Fenton chemistry. BLM·Fe(II) complex possessed a significantly higher catalytic ability than Fe(II) probably because of the further formation of more active “activated oxo-iron-bleomycin complex”. The present method was convenient without any complicated chemical synthesis, modification, or tedious experimental procedures. Analysis results can be seen with the naked eye and monitored by UV-vis spectra. The peak absorbance exhibits a linear relationship with BLM concentrations from 25 nM to 1 μM, and a detection limit of 16 nM can be achieved. The designed colorimetric strategy may provide a promising alternative for BLM detection in clinical samples.
研究领域:
分析化学
·
生物医学
·
临床检验
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DOI
高影响因子
Journal of Materials Chemistry A
·
2017
·Vol. 5
·期 30
·15650-15660
·
IF 8.867
Zhenzhang Weng,Jie Li,Yali Weng,Miao Feng,Zanyong Zhuang,Yan Yu
Current methods that utilize Fenton-like reagents to remove persistent organic pollutants suffer from several limitations, i.e., the reagents may release metal ions into the sludge and cause secondary pollution, the reagents are easily inactivated after use, and the use of additives (e.g., 2KHSO5·KHSO4·K2SO4, Na2S2O8 and H2O2) can be costly but cannot be avoided. In this work, through a one-pot reaction, we prepared surfactant-free porous nano-Mn3O4 as an efficient Fenton-like reagent. Without the addition of external H2O2, it could remove 86.8% and 96.9% of the phenol from an aqueous solution within 1 and 5 min, respectively, and thus outperformed many other reported reagents. The underlying mechanism for the removal of organic pollutants by this Mn3O4 reagent was examined. It was found that the low-valence Mn in Mn3O4 reacted with the dissolved O2 to generate H2O2, and the H2O2 in turn created hydroxyl radicals (HO˙) to degrade organic pollutants. The Mn3O4 was also annealed to generate porous nano-Mn2O3, and a comparison of the performance of Mn3O4 and Mn2O3 in removing organic pollutants revealed that low-valence Mn in the oxides played a critical role in scavenging the pollutants. Note that this novel nano-Mn3O4 could remove pollutants without the addition of external H2O2, and it could be easily reactivated after use through reduction by NaBH4 and thus be recycled. The Mn3O4 can also be successfully applied to complex polluted water containing a mixture of phenolics. These findings pave the way for developing other efficient and environmentally friendly Fenton-like reagents for removing organic pollutants in wastewater.
研究领域:
环境科学
·
材料科学
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DOI
高影响因子
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
·
2017
·Vol. 2017
·期 40
·4797-4802
·
IF 2.444
Yulan Peng,Lingzhi Wang,Yongdi Liu,Haijun Chen,Juying Lei,Jinlong Zhang
Graphical A CoP-decorated g-C 3 N 4 composite catalyst was developed for highly efficient and stable photocatalytic production of H 2 O 2 under visible-light irradiation. The CoP nanoparticles act as a noble metal free cocatalyst for g-C 3 N 4 to enhance the visible-light absorption and promote the separation of photogenerated charge carriers. A composite catalyst combining CoP with g-C 3 N 4 was explored for the photocatalytic production of H 2 O 2 under visible-light irradiation. The composite catalyst was fabricated by growth of CoP nanoparticles on the surface of g-C 3 N 4 . The CoP nanoparticles were well dispersed on the surface of g-C 3 N 4 and could interact with g-C 3 N 4 to improve charge separation and electron transfer. The composite catalyst showed superior catalytic activity compared with pure CoP or g-C 3 N 4 under visible-light irradiation. The optimal catalyst with 1.76 wt.-% CoP loading exhibited the best photocatalytic efficiency with an H 2 O 2 production of 140 µ m in 2 h, which is about 4.6 and 23.3 times those of pure g-C 3 N 4 and pure CoP, respectively. A possible mechanism for the visible-light-driven photocatalytic production of H 2 O 2 is proposed. The composite catalyst exhibited stable performance without obvious loss of catalytic activity after seven successive runs, and thus has good application prospects in sustainable H 2 O 2 production.
研究领域:
材料科学
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环境科学
·
化学
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高影响因子
危险品化学品经营许可证（带存储）