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Innovative Food Science & Emerging Technologies · 2025 · IF 6.8

Investigation of the mechanism of H2O2 combined pulsed electric field treatment reducing the antigenicity of parvalbumin and tropomyosin by high-resolution mass spectrometry, molecular dynamics and DFT computation

Xiangfei Hu,Hui Wang,Qiannan Jiang,Pingwei Wen,Jie Cheng,Haibin Liu,Yueming Hu,Zongcai Tu

The mechanism of H 2 O 2 combined pulsed electric field (PEF) treatment stimulating oxidation and decreasing allergenicity of parvalbumin of grass carp and tropomyosin of king prawn was clarified. Compared to H 2 O 2 treatment alone, the IgG-binding capacity of parvalbumin and tropomyosin significantly decreased by 21.87 % and 81.18 % after H 2 O 2 combined PEF treatment, while the IgE binding capacity reduced by 63.42 % and 76.91 %. •OH caused by electrochemical reaction triggered oxidative degradation of protein and disrupted their allergenic epitopes, which resulted in the structural unfolding, hydrophobic quenching and prevented the recognition by related antibody. Molecular dynamics showed that H 2 O 2 combined PEF treatment promoted •OH interaction with surface residues than alone H 2 O 2 treatment and PEF treatment, where the H 2 O 2 treatment and H 2 O 2 combined PEF treatment caused significant structural alterations of tropomyosin, which greatly converted α-helix to random coil. Furthermore, density functional theory calculation revealed that hydrogen abstraction at C α rendered more stable intermediates where the spin density of the unpaired electron was lower, while alcohol formed by addition of •OH to the side chains was pretty stable but their phenyl and imidazolyl states were more preferred than the saturated side-chains-containing ones.

研究领域: 食品科学 · 生物化学 · 过敏研究 · 生物物理学 · 计算化学
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TALANTA · 2024 · IF 5.6

One-step fabrication of a self-driven point-of-care chip by femtosecond laser direct writing and its application in cancer cell H2O2 detection via semiconductor-based SERS

Yue Wang,Bo Lai,Zhi Yu,Zhangrun Xu

Self-driven microfluidic systems have attracted significant attention and demonstrated great potential in the field of point-of-care (POC) testing due to their device simplicity, low power consumption , increased portability, and reduced sample consumption. To develop POC detection chips with diverse characteristics that meet different requirements, there is a strong demand for feasible strategies that enable easy operation and reduce processing time. Here, a one-step processing approach using femtosecond laser direct writing technology was proposed to fabricate a capillary-actuated POC microfluidic chip. The driving force of the chip is highly dependent on its surface wettability , which can be easily adjusted by changing the laser processing parameters . This POC microfluidic chip allowed for the detection of intracellular H 2 O 2 through a catalytic reaction system that incorporated 5-aminosalicylic acid -sensitized colloidal TiO 2 nanoparticles and horse radish peroxidase , with integrating semiconductor-based surface-enhanced Raman scattering (SERS) quantitative technique. The concentration of H 2 O 2 was determined by the SERS signal of the catalytic products in the microfluidic chip, resulting in rapid detection with minimal sample consumption. Our method provides a simple, feasible, and alternative strategy for POC testing of H 2 O 2 , with a linear range of 10 −2 ∼10 −6  M and a limit of detection of 0.55 μM. This approach was successfully applied to rapid detection of intracellular H 2 O 2 in MCF-7 breast cancer cells with high sensitivity and minimal sample consumption. Additionally, this study not only demonstrates the exceptional advantages of femtosecond laser processing technology in fabricating diverse microfluidic chips for various applications, but also presents an efficient POC testing strategy for detecting cell signaling molecules .

CAS / MDL: 2997-92-4 16561-29-8
研究领域: 微流控技术 · 生物医学工程 · 分析化学 · 癌症研究
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SCIENCE OF THE TOTAL ENVIRONMENT · 2018 · IF 4.61

Efficient removal of several estrogens in water by Fe-hydrochar composite and related interactive effect mechanism of H2O2 and iron with persistent free radicals from hydrochar of pinewood

Jianan Yu,Zhiliang Zhu,Hua Zhang,Ting Chen,Yanling Qiu,Zhaoyi Xu,Daqiang Yin

Recently, hydrochar (HC) with existed persistent free radicals (PFRs) has attracted researches' attention for the potential application in heterogeneous Fenton-like reactions, but studies on the interactive effects of H 2 O 2 , iron, and HC in removal of organic pollutants are still limited. In this paper, magnetic iron (hydr)oxides immobilized hydrochar composite (Fe/HC) derived from hydrothermal carbon (HTC) of pinewood were synthesized and characterized. The interactive effects of H 2 O 2 , iron, and HC in the removal of several estrogens were systematically investigated to understand the removal performance and related mechanism, especially at a pH range close to natural water environment. Batch experiments results showed that estrogens could be efficiently removed over Fe/HC material under a wide pH range of 4–9. Based on the analysis of electron spin resonance, X-ray photoelectron spectroscopy, Mössbauer spectroscopy , and electrochemical impedance spectroscopy, mechanism study indicated that the carbon-centered PFRs on the surface of hydrochar can act as electron donors, and transfer the electrons on adsorbed O 2 to generate O 2 − rapidly, while the addition of H 2 O 2 enhanced the transmission ability of electron to produce OH (ads) on the material surface. The iron and hydrochar components contributed to the desirable removal of estrogens via the synergistic effect between catalysis and adsorption. This study provides a promising application for the use of Fe/HC materials on remediation of pollution with trace estrogens in water environment.

研究领域: 环境科学 · 化学工程
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2018 · IF 11.698

Cu-Al2O3-g-C3N4 and Cu-Al2O3-C-dots with dual-reaction centres for simultaneous enhancement of Fenton-like catalytic activity and selective H2O2 conversion to hydroxyl radicals

Suqian Xu,Hanxu Zhu,Wenrui Cao,Zhibin Wen,Jinnan Wang,Corvini Philippe François-Xavier,Thomas Wintgens

Cu-Al 2 O 3 -g-C 3 N 4 and Cu-Al 2 O 3 -C-dots were synthesized for the first time to enhance the catalytic activity and utilization of H 2 O 2 . SEM, TEM, XPS, FT-IR, XRD, TPR and solid-state EPR were used to characterize the catalysts. In the Cu-Al 2 O 3 -g-C 3 N 4 system, the electron-rich centre of Cu and electron-deficient site of Al were formed due to the higher electronegativity of Cu. Moreover, Cu ions could coordinate with the hydroxyl on the tri-s-triazine ring of g-C 3 N 4 or the graphene conjugated π-domains of C-dots via the Cu O C linkage so that the orbital interactions involving electron transport from π → Cu also induced the formation of an electron-rich Cu centre and an electron-deficient π-electron conjugated system, resulting in the strengthening of the dual-reaction centres. This mechanism was validated by Roman, EPR and XPS spectra. In addition, EPR experiments demonstrated that two electron-transfer processes formed OH in the presence of H 2 O 2 . The first electron transfer was from the electron-rich Cu centres to H 2 O 2 , and the other was from H 2 O to the electron-deficient site. Thus, more OH were generated and high H 2 O 2 utilization was achieved in the Cu-Al 2 O 3 -g-C 3 N 4 and Cu-Al 2 O 3 -C-dots suspension. Furthermore, the turnover frequency (TOF) for the Cu-Al 2 O 3 -C-dots and Cu-Al 2 O 3 -g-C 3 N 4 dispersions were determined and were found to be much higher than those of the classic homogeneous Fenton reaction. Thus, Cu-Al 2 O 3 -g-C 3 N 4 and Cu-Al 2 O 3 -C-dots showed high activity and stability for the catalytic degradation of organic pollutants under mild conditions.

研究领域: 环境科学 · 材料科学
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Journal of Cleaner Production · 2023 · IF 11.1

Engineering low-valence Moδ+ (0<δ<4) sites on MoS2 surface: Accelerating Fe3+/Fe2+ cycle, maximizing H2O2 activation efficiency, and extending applicable pH range in photo-Fenton reaction

Yang Yang,Wenqing Zhen,Tingting Zhao,Maoquan Wu,Shouchun Ma,Liyan Zhao,Jie Wu,Li Liu,Jiaxu Zhang,Tongjie Yao

Fenton/photo-Fenton reaction was limited by slow Fe 3+ /Fe 2+ cycle, low H 2 O 2 activation efficiency, and narrow applicable pH range. Here, Fe atoms doped MoS 2 (Fe–MoS 2 ) with abundant of low-valence Mo δ+ (0 < δ < 4) was prepared. Benefiting from the powerful reduction capacity of Mo δ+ , the rate-limiting step of Fe 3+ reduction was significantly accelerated. Nearly 100% of H 2 O 2 utilization efficiency was realized. Importantly, 90% of H 2 O 2 was effectively activated to be • OH. As a result, tetracycline degradation rate in photo-Fenton reaction catalyzed by Fe–MoS 2 was 5.8 and 4.2 times higher than those of MoS 2 and Fe–MoS 2 -Hyd (prepared by hydrothermal reaction). In comparison with MoS 2 and Fe–MoS 2 -Hyd whose efficient work range were limited in acidic condition, Fe–MoS 2 was a pH-universal catalyst (pH = 2.6–14.0) by taking advantage of the exposed Mo δ+ and photoinduced electrons, largely improving the environmental tolerance. This work simultaneously addressed three bottlenecks in Fenton/photo-Fenton reaction, and provided a new strategy for the preparation of catalysts with powerful catalytic performance and high environmental adaptability.

CAS / MDL: 1317-33-5
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APPLIED SURFACE SCIENCE · 2022 · IF 7.392

In situ-generated H2O2 with NCQDs/MIL-101(Fe) by activating O2: A dual effect of photocatalysis and photo-Fenton for efficient removal of tetracyline at natural pH

Yuanhong Xie,Chenrui Liu,Dejian Li,Yun Liu

Herein, a novel composite of MIL-101(Fe) loaded with nitrogen doped carbon quantum dots (NCQDs/MIL-101(Fe), denoted as NQML), which can construct dual effect of photocatalysis and photo-Fenton for organic pollutants removal, was prepared by solvent impregnation method. Characterization methods proved that NQML had been synthesized successfully. Additionally, the adding volume of NCQDs could effectively influence the photocatalytic activities of NQML-x composites (x represents the adding volume of NCQDs) for tetracycline (TC) degradation, and NQML-8 exhibited the optimum photocatalytic performance among the studied catalysts upon visible light illumination under natural pH, which can completely degrade TC within 180 min. By comparison, the TC degradation kinetic constant in the system with NQML-8 was as 15.85 and 8.24 folds of that in the NCQDs and MIL-101(Fe) systems, respectively. The mechanism study proved that the enhanced photocatalytic performance of NQML was resulted from the visible light up-conversion property, electron-hole separation and transfer capacity of NCQDs. Meanwhile, NQML could not only produce h + but also lead to in-situ generation of O 2 - and H 2 O 2 by activation of O 2 under visible light. The generated H 2 O 2 could react with Fe(II) in MIL-101(Fe) to produce OH so as to construct a dual effect of photocatalysis and photo-Fenton in TC removal.

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CHEMICAL PAPERS · 2022 ·Vol. 76 ·期 5 ·2703-2719 · IF 2.146

Investigation on impact of mutual interactions between elements of Ag nano-particle core-MOF material shell nano-complex and incorporated hemoglobin on electro-catalysis on H2O2 electro-reduction

Sun Ke Wei,Wang Fang,Ma Ting Mei,Zeng Han

Core–shell structure nano-composite made up of Ag nano-wire and metal organic framework material (MOF) was proposed to accommodate Hemoglobin (Hb) molecules. Influences of mutual interactions between Hb and components of core–shell nano-complex on direct electrochemistry and electro-catalytic efficiency on H 2 O 2 reduction of nano-composite with Hb attachment is the main objective of this exploration in this submission. The microscopy, spectrometry and electro-chemical techniques were used to achieve such goal in this paper. The experimental results revealed that the abutting ligation between Hb and Ag nano-wire would lead to the prominent alteration in configuration of heme site in Hemoglobin molecule. However such combination would not increase the active energy of substrate electro-reduction seriously. The quasi-reversible redox process with one proton and single electron participation for Hb-based electrode should be imputed to a typical thin-film confining pattern with normalized rate constant of heterogeneous electron shuttle at 6.6 × 10 –2  s −1 . Mass transferring step of electro-active species in nano-complex with Hb detention (normalized rate at 1.2 × 10 –4  s −1 ) should be regarded as the key factor in restraining the efficiency of enzyme-induced catalysis. Graphical abstract

CAS / MDL: 693-98-1
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ADVANCED FUNCTIONAL MATERIALS · 2025 · IF 19

B Doped Zn Single-Atom Nanozyme With Enhanced Oxidase-Like Activity Combined CRISPR/Cas13a System for RNA Sensing

Shuofeng Li,Fangfang Wang,Chenhuan Wang,Lin Hao,Ningzhao Shang,Pengbo Zhang,Yawen Zhang,Nuo Xiao,Yaai Kang,Jin Liu,Shutao Gao,Chun Wang,Zhi Wang,Qiuhua Wu

Single-atom nanozyme (SAZ) with peroxidase-like activity has attracted great attention in point-of-care (POC) diagnostic, but the use of unstable H 2 O 2 in peroxidase catalytic reactions often leads to low detection accuracy. Thus, developing SAZ with high oxidase (OD)-like activity to construct RNA sensing systems independent of H 2 O 2 is imperative for improving accuracy. Herein, a novel strategy to fabricate boron-nitrogen co-doped zinc SAZ (ZnBNC-SAZ) with excellent OD-like activity by carbonizing Zn based zeolitic boron imidazolate frameworks is reported. The electron deficient B in imidazolate ligand can form Zn─N─B bond in situ during high temperature pyrolysis, which can regulate the electronic structure of Zn and further upshift the d-band center of Zn to improve the OD-like activity. With ZnBNC-SAZ as signal generator, a new method for sensitive RNA detection is developed by combining CRISPR/ cas13 system with terminal deoxynucleotidyl transferase-induced DNA extension reaction. The limits of detection for RNAs are as low as 20 aM. The proposed biosensor is adaptable to a lateral-flow-based readout and is universally applicable for sensing various RNAs by programming the guide RNA. Importantly, the proposed biosensor can monitor the cellular differentiation and identify patients with cervical carcinoma, showing great potential for application in facile POC diagnosis.

研究领域: 纳米技术 · 生物化学 · 分子生物学 · 医学诊断 · 生物医学工程
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ADVANCED FUNCTIONAL MATERIALS · 2024 · IF 18.5

Activatable Janus Nanoparticles for Precise NIR-II Bioimaging and Synergistic Cancer Therapy

Jiasheng Bao,Ruiqi Liu,Zhouyu Yu,Zhen Cheng,Baisong Chang

Despite multifunctional theranostics hold vast potential in deep tissue bioimaging and tumor therapy, activatable nanomedicine with integration of precise diagnosis and effective treatment is usually achieved at the cost of complicated synthesis chemistries. Here, a facile way to design bioresponsive Ag 2 S-Ag Janus probes coated by polyethylene glycol (PEG) (denoted as AAP) is showed, active in the second near-infrared window (NIR-II, 1000–1700 nm). In tumor microenvironment, Ag part can yield hydroxyl radicals (·OH) by consuming H 2 O 2 for high-efficiency chemodynamic therapy (CDT), while Ag 2 S part has impressive photothermal therapy (PTT). The synergistic benefits from Ag and Ag 2 S parts further boosted CDT effect of AAP Janus probes with high photothermal conversion efficiency up to 56.8%. Moreover, multiple lines of evidence supported that extremely faint fluorescence of AAP Janus probes can be significantly activated by overexpressed levels of H 2 O 2 , showing bright NIR-II emission at ≈1270 nm with over 5.6 × 10 3 -fold increase in signal intensity. AAP Janus probes are easily activatable for NIR-II imaging for tumor-specific identification, and effectively ablate tumor tissues with tumor inhibition rate of 96.2%. This study expects that AAP Janus probe will open up a new route to achieve precise tumor diagnosis and treatment in the NIR-II window.

研究领域: 生物医学工程 · 纳米技术 · 癌症治疗 · 生物成像
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SCIENCE OF THE TOTAL ENVIRONMENT · 2024 · IF 8.2

Development and testing of alginate/C3N4porphyrin bead as a self-initiated Fenton photocatalyst for highly efficient atrazine removal

Jiajie Xu,Zhiyu Liu,Tenghui Jin,Xusheng Yang,Huihuang Chen,J. Paul Chen

Fenton reaction has been widely used for efficient treatment of organic wastewater. However, its applications are limited by such key factors as pH < 3. In this study, we developed, tested, and optimized an alginate/C 3 N 4 porphyrin bead (C 3 N 4 por-SA) as a recyclable photocatalyst in a photocatalysis-self-Fenton process to overcome these limitations. Porphyrin-modified C 3 N 4 (C 3 N 4 por) was used as the H 2 O 2 donator, while Fe(III) nodes served as the Fenton reagent . The as-prepared floating alginate/C 3 N 4 por bead utilized the light source as a driving force for the catalysis. Under visible light irradiation for 6 h, the model pollutant atrazine was degraded by 70.96 % by the optimized photocatalyst (named as C 3 N 4 por-SA-Fe1Ca5), demonstrating better photocatalytic performance than alginate/C 3 N 4 beads. This improvement was attributed to the higher H 2 O 2 yield from C 3 N 4 por. The alginate/C 3 N 4 por bead showed better photocatalytic activity even after several consecutive cycles and could easily be recovered for reuse. Furthermore, Fe(III)/Ca(II) bimetallic alginate bead exhibited better photocatalytic activity and a higher content of •OH radicals than the Ca(II) monometallic alginate beads, due to the ability of Fe(III) nodes to serve as a Fenton reagent. The influences of light sources, and commonly existing matters (namely SO 4 2− , Cl − , CO 3 2− , NO 3 − , and humic acid) were investigated. Moreover, the alginate/C 3 N 4 por bead demonstrated good photocatalytic performance in a simulated natural environment without the addition of extra H 2 O 2 , with an atrazine removal percentage of up to 96.3 % after 3-h irradiation. These findings indicated the great potential of alginate/C 3 N 4 por bead in practical applications.

研究领域: 环境科学 · 化学工程 · 材料科学 · 水处理
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY · 2024 · IF 4.3

Robust and sensitive colorimetric detection of glutathione with double-triggering MOF-Fe(DTNB)

Kaining Zhang,Hao Sun,Long Wei,Rui Hu,Hao Liu,Yongchao Lai,Xun Li

Glutathione (GSH) levels have been well validated to correlate with a variety of physiological and pathological conditions, such as malignancy, cardiovascular disease and aging, making the development of accurate, robust and sensitive GSH detection methods highly desirable. In this study, a novel metal–organic framework (MOF-Fe(DTNB))-based colorimetric method with a favorable dual-triggering function was proposed. MOF-Fe(DTNB) exhibits high peroxidase activity, which can catalyze the oxidation of colorless 3,3′,5,5′-tetramethylbenzidine (TMB) to blue ox-TMB by hydrogen peroxide (H 2 O 2 ). This oxidation process of TMB can be inhibited not only by the reducing action of GSH, but also by the thiol exchange reaction between DTNB and GSH, in which the disulfide bond of DTNB in MOF-Fe(DTNB) is cleaved. Thus, with this dual triggering mechanism, the GSH concentration can be robustly measured in the MOF-Fe(DTNB)-derived colorimetric strategy. Significantly, this method is accurate (RSD < 6 %), selective and sensitive in biological plasma samples, with satisfactory recovery rates (96.7–103.3 %). It requires less instrumentation and has less interference from other substances. The linear range of the method is 0–80 µM, and the detection limit is as low as 0.28 µM. This dual-triggering MOF-Fe(DTNB)-derived colorimetric strategy has greatly simplified the GSH detection processes with improved accuracy, in both acidic and basic environments, which has potent applications in biochemical analysis and point-of-care testing.

研究领域: 生物化学 · 分析化学 · 即时检测
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Natural enzyme cascade bimetallic sulfide MoCuSx nanozyme for synergistic photothermal/photodynamic enhanced chemodynamic antimicrobial therapy of wound infection

Caiyun Xu,Junqin Li,Chunlei Ou,Jing Yang,Shuting Fu,Weiqing Hu,Li Wang,Zefeng Wang,Luo Hai,Le Deng,Dinggeng He

Chemodynamic therapy (CDT) involving highly toxic hydroxyl radical (•OH) with no drug resistance has gained widespread attention for antibacterial applications. However, the CDT effect is seriously confined by overexpressed glutathione (GSH) and limited hydrogen peroxide (H 2 O 2 ) in the infection sites. Here, we have constructed a cascade enzyme/nanozyme assembly (MCS/GOx) composing of a bimetallic sulfide MoCuS x (MCS) nanozyme loaded with natural glucose oxidase (GOx) for synergistic photothermal/photodynamic enhanced chemodynamic antimicrobial therapy with high performance. The loaded GOx can promote the peroxidase (POD)-like activity of MCS by providing an acidic microenvironment and self-supplying H 2 O 2 , achieving cascade generation of •OH for efficient CDT. The CDT effect can be further promoted by a co-catalysis mediated by the Mo 4+ /Mo 6+ redox couple. Upon exposure to an 808 nm near-infrared laser, MCS/GOx provides hyperpyrexia for photothermal antibacterial therapy (PTT), and produce singlet oxygen ( 1 O 2 ) for photodynamic therapy (PDT). Moreover, MCS/GOx can significantly consume antioxidant glutathione via the Cu + /Cu 2+ redox couple and PDT-mediated 1 O 2 production, thereby enhancing CDT antibacterial effect. In vitro experiments exhibit that MCS/GOx has combined antimicrobial effect against Staphylococcus aureus and Escherichia coli . Further in vivo studies demonstrate that MCS/GOx can efficiently eliminate bacterial cells in wound tissues and accelerate wound healing with low inflammatory response and good biosafety. Consequently, the proposed MCS/GOx with multiple bactericidal modalities shows a great potential in fighting wound infections.

研究领域: 纳米技术 · 生物医学工程 · 材料科学 · 药学 · 细菌学
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