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WATER RESEARCH · 2015 · IF 5.528

New insights into the primary phototransformation of acetaminophen by UV/H2O2: photo-Fries rearrangement versus hydroxyl radical induced hydroxylation

Shixiang Feng,Xu Zhang,Yanxiang Liu

The phototransformation of acetaminophen (APAP) by UV/H 2 O 2 in deionized water and sewage treatment plant (STP) effluents was studied systematically by a combination of analysis of the reaction intermediates and kinetic study. 1-(2-amino-5-hydroxyphenyl)ethanone ( P1 ) and the reported N -(3,4-dihydroxyphenyl)acetamide ( P2 ) were identified as the main transformation intermediates during the transformation of APAP by UV/H 2 O 2 . There was no influence of OH on the formation kinetics of P1 , while its decay was promoted. The formation and decay kinetics of P2 were accelerated by increases in the concentration of OH. The second-order rate constants for the reaction of OH with APAP, P1 , and P2 were 3.9 × 10 9 , 8.1 × 10 9 , and 4.7 × 10 9  M −1   s −1 , respectively. The kinetic study indicated that the main transformation of APAP also included transformation to 1,4-hydroquinone, although the accumulated concentration of 1,4-hydroquinone was quite low. The presence of anions (Cl − , HCO 3 − / CO 3 2 − , NO 2 − / NO 3 − ), humic acid , commercial drug components or adjuvants, and dissolved organic matters in STP effluents not only changed the transformation kinetics of APAP, but also altered the distribution of the intermediates. The kinetics and pathway of APAP transformation in STP effluent were markedly different from those in deionized water.

CAS / MDL: 665-66-7
研究领域: 环境科学 · 药理学 · 化学动力学
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ACS Applied Bio Materials · 2022 · IF 0

Dual-Ratiometric Fluorescent Probe for H2O2 and HClO in Living Cells and Zebrafish and Application in Alcoholic Liver Injury Monitoring

Peixin Niu,Jiaojiao Liu,Feifei Xu,Lei Yang,Yuhan Li,Ailing Sun,Liuhe Wei,Xingjiang Liu,Xiangzhi Song

Reactive oxygen species (ROS) are an important component for maintaining normal physiological activities in organisms, and abnormal changes in their level are often accompanied by many diseases. As the two most representative components of ROS, HClO and H2O2 play vital roles in many physiological and pathological processes and are interdependent and mutually transformable. Although there is a lot of work that has specifically detected HClO or H2O2, there are few reports on the simultaneous differential detection of HClO and H2O2. Here, we report a ratio-based fluorescent probe capable of simultaneously distinguishing HClO and H2O2 based on making the best use of the untapped potential of coumarin derivatives. This probe was triumphantly put into use in the discriminative identification of HClO and H2O2 in aqueous media with high sensitivity and selectivity, and the probe was appropriate in a wide pH range. Furthermore, the imaging experiment for HClO and H2O2 in cells and zebrafish was eventually proven to be feasible. Importantly, this probe was qualified for monitoring the variation of HClO and H2O2 levels in organisms with alcoholic liver injury.

研究领域: 生物化学 · 医学 · 分析化学
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Journal of Environmental Sciences · 2024 · IF 5.9

Assessing the effectiveness and mechanisms of Fe/PS, Fe/H2O2, and O3 treatment for water disinfection: Spotlight on VBNC bacteria

Zheng Qi,Zaihui Huang,Chunguang Liu

Advanced oxidation processes (AOPs) exhibit significant potential for water disinfection due to their generation of large quantities of highly oxidizing free radicals. However, the neglect of viable but nonculturable (VBNC) cells obscures their true disinfection efficacy and potential environmental health risks. Therefore, the study evaluated the disinfection effectiveness and mechanisms of typical AOPs, including Fe/H 2 O 2 , Fe/persulfate (PS), and O 3 , from the perspective of the production of VBNC bacteria. The results indicate that Fe/PS exhibits the strongest bacterial inactivation rate (99.94%), and the cells lose their ability to reactivate. Fe/H 2 O 2 and O 3 induce more cells to enter the VBNC state compared to Fe/PS. Moreover, different AOPs result in varying levels of free radical production and utilization efficiency, with SO 4 •− and O 3 exhibiting greater selectivity in deactivating bacteria compared to HO • . The inhibition of VBNC bacteria production by Fe/PS treatment may be attributed to the combined action of HO • and SO 4 •− on microorganisms, leading to oxidative stress and metabolic disruption in bacteria through the inhibition of biofilm formation and aminoacyl-tRNA biosynthesis ( p < 0.05), thereby causing direct bacterial death rather than entry into the VBNC state. In contrast, Fe/H 2 O 2 and O 3 result in the upregulation of the metabolism of alanine, aspartate, and glutamate, as well as styrene degradation capacity by the bacteria, leading to the production of more VBNC bacteria. Overall, the study offers insights into mitigating potential biological risks in water disinfection and developing environmentally friendly and efficient disinfection technologies.

研究领域: 环境科学 · 微生物学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2025 · IF 9

CdS/TpPa-Cl2/MXene hybrids with chlorine-mediated MXenes and CdS for photocatalytic H2O2 production in ambient air and pure water

Guanglu Xia,Jianhao Qiu,Shengwang Gong,Dingliang Dai,Biyao Fang,Yixin Li,Jianfeng Yao

Specific intermolecular interactions are the keys to constructing benign interfacial compatibility, which determines the activities of hybrid photocatalysts. In this study, CdS/TpPa-Cl 2 /MXene hybrids were compactly developed through the mediation of chlorine groups in TpPa-Cl 2 with MXenes and CdS. Owing to the formation of the Schottky junction between TpPa-Cl 2 and MXene and the heterojunction between TpPa-Cl 2 and CdS, as well as the close interfacial contacts among them, the photogenerated electron–hole pairs are effectively separated, which ultimately results in efficient photocatalytic activities. For visible-light-driven H 2 O 2 production in ambient air and pure water, CdS/TpPa-Cl 2 /MXene hybrids could achieve a high H 2 O 2 yield of 1005 μmol·L –1 , which is 2.5, 9.7 and 6.5 times greater than those of pure TpPa-Cl 2 , MXene and CdS, respectively. The mechanism investigation revealed that an indirect O 2 reduction pathway with ·O 2 – as an intermediate occurred for H 2 O 2 production over the CdS/TpPa-Cl 2 /MXene composites, and this two-electron O 2 reduction process was manifested as the primary way. This study provides insight into the construction of multi-component composite photocatalysts with high efficiency on the basis of covalent organic frameworks.

研究领域: 材料科学 · 环境科学 · 化学
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Journal of Materials Chemistry B · 2018 ·Vol. 7 ·期 2 ·296-304 · IF 4.776

Metal-doped carbon nanoparticles with intrinsic peroxidase-like activity for colorimetric detection of H2O2 and glucose

Yan-Wen Bao,Xian-Wu Hua,Huan-Huan Ran,Jia Zeng,Fu-Gen Wu

Nanomaterial-based enzyme mimics (nanozymes) are attracting increasing attention because of their low production cost, high stability against denaturation, and resistance to high concentrations of substrates. Here, carbon nanoparticles doped with a small amount (<5 mol%) of Pt (denoted as PtCNPs) are synthesized via a facile, cost-effective hydrothermal treatment of p-phenylenediamine (PPD) and K2PtCl4. The obtained PtCNPs possess high aqueous stability, excellent water-dispersibility, and suitable size (∼15 nm). More interestingly, the PtCNPs exhibit an intrinsic peroxidase-like activity that can quickly catalyze 3,3′,5,5′-tetramethylbenzidine (TMB) in the presence of hydrogen peroxide (H2O2) and produce a blue color. Importantly, since satisfactory catalytic properties were also observed when K2PtCl4 was replaced with CuCl2, NiCl2, or Na2PdCl4 during the synthesis, the PPD- and inorganic metal salt-involved hydrothermal synthetic approach may be developed as a general and simple way to fabricate new nanozymes. Besides, the steady-state kinetics reveals that the PtCNPs have a stronger affinity for TMB and a weaker affinity for H2O2 compared with horseradish peroxidase. On the basis of the color reaction, a colorimetric detection method for H2O2 and glucose has been successfully established with a detection limit of 0.15 and 0.30 μM, respectively. Further, the method has also been successfully applied for glucose detection in human serum samples. To sum up, this work develops a new synthetic method of metal-doped carbon nanomaterials and demonstrates their capability for the sensitive and selective detection of H2O2 and glucose, which may foster the development of new nanozymes for biosensing applications.

研究领域: 纳米生物学 · 生物传感 · 酶学
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY · 2020 · IF 3.232

Platinum (II)-doped graphitic carbon nitride with enhanced peroxidase-like activity for detection of glucose and H2O2

Guo Zeng,Minghui Duan,Yifan Xu,Fahuan Ge,Weiguo Wang

A platinum (II)-doped graphitic carbon nitride (Pt 2+ @g-C 3 N 4 ) nanozyme was prepared in this work. Compared to g-C 3 N 4 , Pt 2+ @g-C 3 N 4 shows enhanced peroxidase-like activity. According to DFT calculations and ESR measurements, the Pt on the surface of g-C 3 N 4 accelerates the decomposition of H 2 O 2 into OH and consequently accelerates TMB oxidation. Furthermore, as a proof of concept, the obtained Pt 2+ 2.30 @g-C 3 N 4 was applied in the detection of glucose with an LOD of 0.01 mM. The reproducibility and precision tests of the glucose detection method based on Pt 2+ 2.30 @g-C 3 N 4 show that this method is reliable and feasible for the detection of glucose.

研究领域: 生物化学 · 材料科学 · 分析化学
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RSC Advances · 2014 ·Vol. 4 ·期 67 ·35500-35504 · IF 3.708

CoxFe3−xO4 hierarchical nanocubes as peroxidase mimetics and their applications in H2O2 and glucose detection

Wenshu Yang,Jinhui Hao,Zhe Zhang,Baoping Lu,Bailin Zhang,Jilin Tang

A facile approach was proposed for the synthesis of hierarchical CoxFe3−xO4 nanocubes (CF nanocubes), using Prussian Blue (PB) as precursor. The method consists of the synthesis of hierarchical cobalt–iron Prussian blue analogues (PBAs) through the reaction of PB nanocubes with CoCl2 in a water bath and subsequently calcining the corresponding PBA precursor. The obtained CF nanocubes were characterized using transmission electron microscopy, scanning electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy and N2 adsorption–desorption isotherm measurements. It is found that the hierarchical CF nanocubes have a large specific surface area (108 m2 g−1). Considering the hierarchical structure and the doping of Co in Fe3O4 are beneficial for the catalytic activity of the catalyst, an efficient and simple colorimetric biosensor for H2O2 and glucose was fabricated using CF nanocubes as a peroxidase mimetic. The good catalytic activity and low-cost make the hierarchical CF nanocubes a useful biocatalyst for a wide range of potential applications in medicine and biotechnology.

CAS / MDL: 9001-37-0 54827-17-7
研究领域: 生物传感 · 材料科学 · 医学诊断
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2022 · IF 9.965

Protonated g-C3N4 coated Co9S8 heterojunction for photocatalytic H2O2 production

Han Zhang,Xuefeng Bai

Photocatalytic H 2 O 2 production is an eco-friendly technique because only H 2 O, molecular O 2 and light are involved. However, it still confronts the challenges of the unsatisfactory productivity of H 2 O 2 and the dependence on organic electron donors or high purity O 2 , which restrict the practical application. Herein, we construct a type-II heterojunction of the protonated g-C 3 N 4 coated Co 9 S 8 semiconductor for photocatalytic H 2 O 2 production. The ultrathin g-C 3 N 4 uniformly spreads on the surface of the dispersed Co 9 S 8 nanosheets by a two-step method of protonation and dip-coating, and exhibits improved photogenerated electrons transportability and e - -h + pairs separation ability. The photocatalytic system can achieve a considerable productivity of H 2 O 2 to 2.17 mM for 5 h in alkaline medium in the absence of the organic electron donors and pure O 2 . The optimal photocatalyst also obtains the highest apparent quantum yield (AQY) of 18.10% under 450 nm of light irradiation, as well as a good reusability. The contribution of the type-II heterojunction is that the migrations of electrons and holes within the interface between g-C 3 N 4 and Co 9 S 8 matrix promote the separation of photocarriers, and another channel is also opened for H 2 O 2 generation. The accumulated electrons in conduction band (CB) of Co 9 S 8 contribute to the major channel of two-electron reduction of O 2 for H 2 O 2 production. Meanwhile, the electrons in CB of g-C 3 N 4 participate in the single electron reduction of O 2 as an auxiliary channel to enhance the H 2 O 2 production.

研究领域: 材料科学 · 环境科学 · 化学
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Nature Communications · 2024 ·Vol. 15 ·期 1 ·1-12 · IF 14.7

A metal-free cascaded process for efficient H2O2 photoproduction using conjugated carbonyl sites

He Tiwei,Tang Hongchao,Wu Jie,Wang Jiaxuan,Zhang Mengling,Lu Cheng,Huang Hui,Zhong Jun,Cheng Tao,Liu Yang,Kang Zhenhui

Carbon-based metal-free catalysts are promising green catalysts for photocatalysis and electrocatalysis due to their low cost and environmental friendliness. A key challenge in utilizing these catalysts is identifying their active sites, given their poor crystallinity and complex structures. Here we demonstrate the key structure of the double-bonded conjugated carbon group as a metal-free active site, enabling efficient O 2 photoreduction to H 2 O 2 through a cascaded water oxidation − O 2 reduction process. Using ethylenediaminetetraacetic acid as a precursor, we synthesized various carbon-based photocatalysts and analyzed their structural evolution. Under the polymerization conditions of 260 °C to 400 °C, an N -ethyl- 2 -piperazinone-like structure was formed on the surface of the catalyst, resulting in high photocatalytic H 2 O 2 photoproduction (2884.7 μmol g −1 h −1 ) under visible light. A series of control experiments and theoretical calculations further confirm that the double-bond conjugated carbonyl structure is the key and universal feature of the active site of metal-free photocatalysts.

CAS / MDL: 637-88-7
研究领域: 材料科学 · 催化 · 光化学
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2023 · IF 8.2

Pd nanoparticles stabilized by bitter gourd polysaccharide with peroxidase properties for H2O2 detection

Ruyu Li,Yu Zhao,Tingting Zhang,Zejin Ju,Xianbing Ji,Yanshuai Cui,Longgang Wang,Haiyan Xiao

The development of nanozymes using noble metal nanoparticles to replace natural peroxidase in bio-related detection has been gain great interest. Noble metal nanoparticles with small size have large specific surface area. However, small noble metal nanoparticles tend to aggregate without stabilizer. In this paper, small Pd nanoparticles (3–6 nm) stabilized by bitter gourd polysaccharide (Pd n -BGP NPs) were prepared by using bitter gourd polysaccharide as reducing agent and stabilizing agent. Pd 25 -BGP NPs had peroxidase-like catalytic property. And the catalytic kinetics of Pd 25 -BGP NPs towards substrates conformed to the Michaelis-Menten equation. Furthermore, a method was established to detect H 2 O 2 using Pd 25 -BGP NPs. The linear range and detection limit of this method was 20–320 μM and 2.04 μM, respectively. Finally, Pd 25 -BGP NPs had good biocompatibility when the concentration was less than 80 μg/mL. The prepared Pd nanoparticles with high stability showed their good prospect in H 2 O 2 detection.

研究领域: 纳米技术 · 生物化学 · 分析化学 · 材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2019 · IF 5.107

Degradation effect and mechanism of gas-liquid phase dielectric barrier discharge on norfloxacin combined with H2O2 or Fe2+

Zimu Xu,Xiaojuan Xue,Shuheng Hu,Yunxia Li,Jie Shen,Yan Lan,Rongxing Zhou,Fan Yang,Cheng Cheng

Norfloxacin (NOR) is a typical kind of Fluoroquinolone antibiotics which is extensively used around the world. Residues of NOR have been found continuously increasing in the water systems thus posing detrimental effects to the aquatic ecosystem and human health. In this study, the degradation effect and mechanism on NOR in aqueous solution are investigated by gas-liquid phase dielectric barrier discharge (DBD) plasma combined with different catalysts (H 2 O 2 or Fe 2+ ). The concentrations of three representative plasma-generated long-lived reactive species (H 2 O 2 , O 3 and N O 3 - NO3- ) were measured in dH 2 O and found enhancing with the lengthening discharge period. Variations on the treatment parameters were carried out in discharge power, initial solution pH and the concentration of catalysts. A discharge power at 60 W provided optimal balance on the degradation effect and energy efficiency would be beneficial, while there is not much impact from the initial solution pH on NOR degradation. Both H 2 O 2 and Fe 2+ at low concentration (0.5–10 mg/L of Fe 2+ , 0.1–1.0 mmol/L of H 2 O 2 ) were observed contributing to the improvement on the NOR degradation rate, while inhibition would occur at high concentration (10–20 mg/L of Fe 2+ , 1.0–2.0 mmol/L of H 2 O 2 ). The DBD/H 2 O 2 (0.5 mmol/L)/Fe 2+ (10 mg/L) system was found the optimal condition to achieve a high NOR degradation rate of more than 98% after plasma treatment for only 0.5 min at discharge power of 60 W. Moreover, 72.3 ± 1.7% of the total organic carbon (TOC) in NOR solution have been removed in the DBD/Fe 2+ (10 mg/L) system at 15 min which signifies a high mineralization efficiency. The cleavage of piperazine ring and quinolone ring, defluorination and hydroxylation are considered the major pathways for NOR degradation. The biological toxicity of the plasma/Fe 2+ -induced degradation intermediates has been detected and it fluctuated with the treatment time and finally declined. Therefore, the DBD/catalyst system could be an effective and promising method on pharmaceutical wastewater treatment in the future.

CAS / MDL: 75-05-8 67-56-1
研究领域: 环境科学 · 水处理技术
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MICROCHEMICAL JOURNAL · 2022 · IF 5.304

Dual enzyme-mimicking fluorescent amino terephthalic acid/CuFe/adenosine triphosphate nanoparticles for determination of H2O2 and ascorbic acid

Zhiwen Gan,Tian Zhang,Xuanxuan An,Qin Tan,Shujun Zhen,Yongmei Hu,Xiaoli Hu

Many nanozymes have been synthesized, though, it is still necessary to rationally synthesize multifunctional nanozymes for diverse applications. Herein, we fabricate three fluorescent nanozymes with peroxidase- and laccase-like activities under moderate conditions. Three nanozymes, NH 2 BDC/CuFe/ATP (NPs-1), NH 2 BDC/CuFe/ADP (NPs-2), NH 2 BDC/CuFe/AMP (NPs-3), are constructed based on three adenosine phosphates coordinated transition metal ions (Cu 2+ and Fe 3+ ) and adsorbing fluorescent amino terephthalic acid (NH 2 -BDC). They exhibit different laccase-like activity, which may result from the difference in steric configurations of nanozymes. Among them, NPs-1 possesses high peroxidase-mimicking activity and stability. Interestingly, o-phenylenediamine (OPD) is oxidized to 2,3-diaminophenazine (DAP) by ·OH which NPs-1 catalyzes H 2 O 2 to produce. The fluorescence of NPs-1 ( λ em  = 445 nm) is effectively reduced based on the inner filter effect between DAP and NPs-1, which recovers after adding AA. Based on stable fluorescence and high peroxidase-like activity of NPs-1, a system for determining H 2 O 2 and AA is established in linear ranges of 2.0–200.0 and 4.0–300.0 μmol L −1 with limits of detection of 1.82 and 2.92 μmol L −1 . The fluorescent probe shows a good performance in detecting AA in real samples. Furthermore, NPs-1 is applied in smartphone-based detection of AA by measuring its intrinsic fluorescence. This work provides a facile strategy for the design of multi-functional nanozymes.

研究领域: 生物化学 · 分析化学 · 纳米技术
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