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Journal of Materials Chemistry B · 2024 · IF 6.1

Enzyme-triggered on-demand release of a H2O2-self-supplying CuO2@Fe3O4 nanoagent for enhanced chemodyamic antimicrobial therapy and wound healing

Sijie Zhang,Sameer Hussain,Yuhai Tang,Kaili Wang,Xingyan Wang,Long Zhang,Yuheng Liao,Chen Wang,Yi Hao,Ruixia Gao

Nanoagents for chemodynamic therapy (CDT) hold a promising future in the field of antimicrobials, especially copper peroxide (CuO2) (CP) nanomaterials which have garnered significant attention due to their ability to self-supply H2O2. Nevertheless, the poor stability of CuO2 remains a critical challenge which restricts its practical application in the antibacterial field. In this study, an advanced nano-antimicrobial system HA-CP@Fe3O4 with enzyme-responsive properties is developed by coating hyaluronic acid (HA) on CuO2-loaded iron tetraoxide nanoparticles. The coating of HA not only stabilizes the CuO2 nanomaterials but also provides responsiveness towards the enzyme hyaluronidase, which is typically secreted by some bacteria. The outer layer of HA in HA-CP@Fe3O4 undergoes decomposition in the presence of hyaluronidase-secreting bacteria, resulting in the release of CuO2@Fe3O4. The released CuO2@Fe3O4 then self-supplies H2O2 and generates reactive oxygen species (ROS) within the infected microenvironment through Fenton and Russell effects, to ultimately achieve effective and precise antimicrobial activity. Simultaneously, the magnetic property provided by Fe3O4 allows the substance to be directed towards the infection site. Both in vitro and in vivo tests demonstrated that HA-CP@Fe3O4 exhibited excellent antimicrobial capabilities at low concentration (30 μg mL−1), exceptional biocompatibility and the ability to accelerate wound healing. The findings of this work offer a new and promising approach for targeted and precise CDT.

研究领域: 纳米技术 · 生物医学工程 · 抗菌治疗 · 伤口愈合 · 材料科学
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CHEMOSPHERE · 2019 · IF 5.108

Construction of Ti3+-TiO2-C3N4por compound coupling photocatalysis and Fenton-like process: Self-driven Fenton-like process without extra H2O2 addition

Jiajie Xu,Guodong Dai,Biyu Chen,Donglin He,Yue Situ,Hong Huang

An efficient heterogeneous photocatalytic process coupling photocatalysis and Fenton-like process was carried out, where the Fenton-like cycle could be driven by self-produced H 2 O 2 rather than extra H 2 O 2 addition. It was revealed that C 3 N 4 por exhibited good performance at H 2 O 2 production in pure water, which was enhanced up to eight times than bare g-C 3 N 4 . Fenton-like cycle was constructed in Ti 3+ -TiO 2 -C 3 N 4 por as C 3 N 4 por severed as H 2 O 2 donator, while the Ti 3+ -TiO 2 was able to provide photoinduced electrons for the Fenton-like process, resulting in the generation of much more OH radical. In addition, ESR spectra were performed to confirm the promotion of the Fenton-like cycle and much more OH radical was detected in Ti 3+ -TiO 2 -C 3 N 4 por than Ti 3+ -TiO 2 -C 3 N 4 due to the great improvement in H 2 O 2 production of C 3 N 4 por. What’s more, the feasible photocatalytic mechanism of Ti 3+ -TiO 2 -C 3 N 4 por composite was also proposed.

研究领域: 环境科学 · 材料科学
✓ 已验证 DOI PubMed 高影响因子
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Journal of Breath Research · 2019 ·Vol. 13 ·期 3 ·036005 · IF 3

Effect of H2O2 induced oxidative stress (OS) on volatile organic compounds (VOCs) and intracellular metabolism in MCF-7 breast cancer cells

Yuanling Liu,Wenwen Li,Yixiang Duan

Oxidative stress (OS) refers to the process of oxidative damage caused by reactive oxygen species (ROS) and reactive nitrogen species (RNS) accumulated by the organisms or cells during the process of generating and scavenging oxygen free radicals. In this study, an OS model of MCF-7 cells was constructed through H2O2-treatment, which for the first time combined volatile organic compounds (VOCs) and intracellular metabolic analysis for a comprehensive and in-depth study of the OS effect on cell metabolism. The VOCs produced by cells in H2O2-treated groups and control groups were extracted with solid-phase microextraction (SPME) and analyzed by gas chromatography-mass spectrometer (GC-MS). Meanwhile, the intracellular metabolites were extracted by methanol and analyzed by GC-MS coupled with silyl-derivatization. The results indicated 15 VOCs and 29 intracellular metabolites were statistically different (p < 0.05) between the H2O2-treated groups and the control groups. The VOC biomarkers were mainly linear chain alkanes and branched chain alkanes, and they were up-regulated in cells treated by H2O2. The intracellular metabolites with significant changes were mainly fatty acids, amino acids, and organic acids. Most of them, however, were down-regulated under OS state. This study revealed volatile and non-volatile metabolites that influenced by elevated OS in MCF-7 cells, and provided clues for mechanism exploration of exhaled biomarkers, thus promoting the non-invasive prediction of BC.

研究领域: 癌症研究 · 代谢组学 · 生物化学
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY · 2017 ·Vol. 164 ·期 4 ·B92 · IF 3.259

Facile Synthesis of a Nickel Sulfide (NiS) Hierarchical Flower for the Electrochemical Oxidation of H2O2 and the Methanol Oxidation Reaction (MOR)

Jingchao Zhang,Chunying Xu,Daojun Zhang,Jingli Zhao,Shuxian Zheng,Huimin Su,Feifei Wei,Baiqing Yuan,Carlos Fernandez

The synthesis of a novel hierarchical flower-like NiS via a solvothermal method for the electrochemcial oxidation of H2O2 on a carbon paste electrode with high catalytic activity for the (MOR) in an alkaline medium has been reported. Novel nickel sulfide (NiS) hierarchical flower-like structures were characterized by X-ray diffraction, scanning electron microscope, and transmission electron microscopy. A carbon paste electrode was modified with the as-prepared hierarchical flower-like NiS, resulting in a high electrocatalytic activity toward the oxidation of H2O2. The NiS-modified electrode was used for H2O2 sensing, which was achieved over a wide linear range from 0.5 μM to 1.37 mM (I/μA = −0.19025 + 0.06094 C/mM) with a low limit of detection (LOD) of 0.3 μM and a limit of quantitation (LOQ) of 0.8 μM. The hierarchical flower-like NiS also exhibited a high electrocatalytic activity for the methanol oxidation reaction (MOR) in an alkaline medium with a high tolerance toward the catalyst-poisoning species generated during the MOR. The MOR proceeded via the direct electrooxidation of methanol on the oxidized NiS surface layer because the oxidation peak potential of the MOR was more positive than that of the oxidation of NiS.

研究领域: 材料科学 · 电化学 · 分析化学
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Nanoscale · 2020 ·Vol. 12 ·期 42 ·21674-21686 · IF 6.895

Carbon nanocage-based nanozyme as an endogenous H2O2-activated oxygenerator for real-time bimodal imaging and enhanced phototherapy of esophageal cancer

Jingjing Liu,Jiameng Gao,Amin Zhang,Yuliang Guo,Shanshan Fan,Yu He,Kai Yang,Jianbo Wang,Daxiang Cui,Yingsheng Cheng

Intelligent phototherapy by theranostic nanosystems that can be activated by a tumor microenvironment has high sensitivity and specificity. However, hypoxia and low drug accumulation in tumors greatly limit its clinical application. Herein, we have designed a cage-like carbon-manganese nanozyme, which effectively relieves tumor hypoxia and delivers numerous photosensitizers (PSs) to the tumor site, for real-time imaging and enhanced phototherapy of esophageal cancer. Specifically, bovine serum albumin (BSA) was used as a template and reducing agent for preparing a BSA-MnO2 nanozyme; then a BSA-MnO2/IR820@OCNC (BMIOC) nanosystem was successfully synthesized by crosslinking BSA-MnO2 on the surface of IR820-loaded carboxylated carbon nanocages (OCNCs). Abundant PSs were successfully delivered to tumor sites via hollow OCNCs, and the final loading rate of IR820 reached 42.8%. The intratumor BMIOC nanosystem can be initiated by a tumor microenvironment to switch on its magnetic resonance (MR) imaging signal, and photothermal therapy (PTT) and photodynamic therapy (PDT) functions. Notably, the BSA-MnO2 nanozyme, with intrinsic catalase (CAT)-like activity, catalyzed endogenous H2O2 for oxygen generation to overcome tumor hypoxia and enhance PDT, thereby leading to more efficient therapeutic effects in combination with OCNC-elevated PTT. In addition, the H2O2-activated and acid-enhanced properties enable our nanosystem to be specific to tumors, protecting normal tissues from damage. By integrating a high drug loading capacity, a hypoxia regulation function, an enlarged phototherapy effect, and bimodal imaging into a nanozyme-mediated nanoreactor, this work realizes a “one for all” system and represents promising clinical translation for efficient esophageal cancer theranostics.

研究领域: 纳米医学 · 癌症治疗 · 医学影像 · 生物医学工程
✓ 已验证 DOI PubMed 高影响因子
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Mechanism insights into H2O2 in situ generation and activation for ciprofloxacin degradation by electro-peroxidation using the ACF@RuO2/Ti cathode

Songyu Ren,Aimin Wang,Yanyu Zhang,Yongjun Song,Zhenjun Wen,Zhongguo Zhang

Electrocatalytic H 2 O 2 production via the two-electron oxygen reduction reaction on the cathode surface plays a crucial role in the electro-peroxidation (EO-H 2 O 2 ). In this work, the H 2 O 2 generation potential of the EO-H 2 O 2 process using an activated carbon fiber attached RuO 2 /Ti cathode (ACF@RuO 2 /Ti) was evaluated by simulation experiments with a high-precision syringe pump. Results shown that the actual average H 2 O 2 accumulation rate reached up to 4.92 mg h −1 cm −2 , while more than 95 % of the electrogenerated H 2 O 2 was decomposed quickly. Electron paramagnetic resonance and quenching tests confirmed that the primary oxidant • OH was produced from H 2 O 2 activation by ACF, RuO 2 catalyst and their synergistic effect, while RuO 2 played dominant role. The production of • OH in the EO-H 2 O 2 process was also confirmed by the degradation and mineralization of antibiotic ciprofloxacin. The characterization results indicated that heterogeneous catalysis of cathode was due to both the pyridinic nitrogen and oxygen-containing groups of ACF, along with RuO 2 catalyst on the RuO 2 /Ti surface. This study provides new insights into the mechanisms of the in situ H 2 O 2 generation and activation in the EO-H 2 O 2 process.

CAS / MDL: 3317-61-1 98-00-0
研究领域: 环境科学 · 电化学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Selective photocatalytic remediation of para-substituted phenol pollutants over iodine-doped Bi2MoO6 via in-situ generated H2O2 and iodine radicals activation

Haotian Liu,Chuang Wang,Yi Yang,Minghui Gao,Aifang Xue,Hao Chen,Xing Ding

The preferential degradation of specific harmful organic pollutants in photocatalytic processes is critically important, yet remains a significant challenge due to the uncontrolled nature of reactive species, particularly those with high oxidation potentials such as •OH and h + . In this work, we designed an iodine-doped Bi 2 MoO 6 semiconductor to establish a system for photo-induced H 2 O 2 generation. The incorporation of iodine led to a steady enhancement in the selective photo-degradation of para -substituted phenolic pollutants, known precursors to carcinogenic p-benzoquinones, facilitated by the activation of iodine radicals through H 2 O 2 . This system exhibited impressive photo-degradation (96 %) and mineralization efficiency for acetaminophen (APAP), along with superior environmental applicability. It also demonstrated selectivity in degrading phenols with para -substitutions. The in-situ generation and activation of H 2 O 2 and •I were identified as the crucial pathways in this photocatalytic system. This work provides a novel modification path to accomplish the simultaneous generation and utilization of H 2 O 2 in the photocatalytic system and ultimately makes a remarkable performance for the targeted remediation of environmental pollutants.

研究领域: 环境科学 · 光催化材料 · 污染治理
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APPLIED SURFACE SCIENCE · 2024 · IF 6.3

H2O2-assisted room temperature preparation of crystalline TiO2 and Ti3C2Tx-derived C-doped amorphous TiOx homojunction for photocatalytic degradation of tetracycline

Junhao Cai,Yaru Peng,Po Hu,Yuan Zhou,Qiaoge Yao,Hao Lyu,Youtang Gao

The light absorption, active sites, and charge carriers separation of photocatalysts are extremely important factors in the field of photocatalysis. Near-perfect lattice-matched homojunction constructed using disorder engineering and doping strategies is an effective strategy to improve photocatalytic activity. Herein, we developed crystalline TiO 2 nanoparticles (NPs) and Ti 3 C 2 T x MXene-derived C-doped amorphous TiO x homojunction (TCT) at room temperature. In this homojunction, TiO 2 NPs are evenly distributed on the surface of the C-TiO x nanosheet to form a type-II structure, which promotes the separation of photogenerated carriers. The light absorption range of TCT extends to 550 nm due to the presence of intermediate energy levels in C-TiO x , which increases its photon absorption capacity. Moreover, TCT possesses a large number of oxygen vacancies, which are beneficial for improving the adsorption and degradation of pollutants. These characteristics of TCT could significantly improve its photodegradation performance for tetracycline. Interestingly, the precursor mass ratio of TCT with the best degradation efficiency is different under different illumination conditions, which is attributed to the different band gaps of C-TiO x and TiO 2 NPs resulting in different light absorption ranges. This work provides a new approach to rationally designing crystalline and amorphous homojunction for photocatalytic applications.

研究领域: 材料科学 · 环境科学
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Journal of Materials Chemistry B · 2024 ·Vol. 12 ·期 25 ·6164-6174 · IF 6.1

H2O2/acid self-supplying double-layer electrospun nanofibers based on ZnO2 and Fe3O4 nanoparticles for efficient catalytic therapy of wound infection

Lihui Yuwen,Pei Lu,Qi Zhang,Kaili Yang,Zhaowei Yin,Bin Liang,Lianhui Wang

Catalytic therapy based on nanozymes is promising for the treatment of bacterial infections. However, its therapeutic efficacy is usually restricted by the limited amount of hydrogen peroxide and the weak acidic environment in infected tissues. To solve these issues, we prepared polyvinyl alcohol (PVA)–polyacrylic acid (PAA)–iron oxide (Fe3O4)/polyvinyl alcohol (PVA)–zinc peroxide (ZnO2) double-layer electrospun nanofibers (PPF/PZ NFs). In this design, PVA serves as the carrier for ZnO2 nanoparticles (NPs), Fe3O4 NPs, and PAA. The double-layer structure of nanofibers can spatially separate the PAA and ZnO2 to avoid their reaction with each other during preparation and storage, while in the wet wound bed, PVA can dissolve and PAA can provide H+ ions to promote the generation of hydrogen peroxide and subsequent conversion to hydroxyl radicals for bacteria killing. In vitro experimental results demonstrated that PPF/PZ NFs can reduce the methicillin-resistant Staphylococcus aureus by 3.1 log (99.92%). Moreover, PPF/PZ NFs can efficiently treat the bacterial infection in a mouse wound model and promote wound healing with negligible toxicity to animals, indicating their potential use as “plug-and-play” antibacterial wound dressings. This work provides a novel strategy for the construction of double-layer electrospun nanofibers as catalytic wound dressings with hydrogen peroxide/acid self-supplying properties for the efficient treatment of bacterial infections.

研究领域: 生物材料学 · 医学 · 纳米医学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2024 · IF 8.1

Graphene quantum dot @ Flower-like Bi2S3 composites for photodegradation of organic pollutants combined photosynthesis of H2 and H2O2 from treated water

Jingjing Wang,Ruonan Liu,Yuxin Qiao,Shuxin Liu,Chuanguang Qin

In this work, flower-like Bi 2 S 3 was prepared by hydrothermal method using different solvents, and materials with better performance were selected. Graphene quantum dots (GQD, which is rich in specific amino groups) was prepared by aqueous phase fusion technology. Ultimately, a straightforward one-step hydrothermal process was used to successfully manufacture composite materials in order to build GQD(4)/Bi 2 S 3 heterostructures. The study results have shown that the H 2 production efficiency of 2% GQD(4)/Bi 2 S 3 is the best, and its photocatalytic hydrogen production efficiency within 3 h is 5.92 times that of GQD(4) and 3.03 times that of Bi 2 S 3 . The H 2 O 2 production and tetracycline (TC) degradation efficiency of 2% GQD(4)/Bi 2 S 3 are the best, while the methylene blue (MB) degradation efficiency of 1% GQD(4)/Bi 2 S 3 is relatively better. The research results show that as a perfect combination of GQD(4)/Bi 2 S 3 heterostructures, it offers a productive plan for eliminating organic pollutants in water and producing clean oxidant and hydrogen energy.

CAS / MDL: 10035-06-0
研究领域: 材料科学 · 环境科学 · 能源科学
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ACTA PHYSICO-CHIMICA SINICA · 2025 · IF 13.5

Femtosecond transient absorption spectroscopy investigation on ultrafast electron transfer in S-scheme ZnO/CdIn2S4 photocatalyst for H2O2 production and benzylamine oxidation

Yi Yang,Xin Zhou,Miaoli Gu,Bei Cheng,Zhen Wu,Jianjun Zhang

Photocatalytic hydrogen peroxide (H 2 O 2 ) production is a crucial process for clean energy conversion, involving the reduction of O 2 through two electrons. However, this process is often hampered by the sluggish water oxidation involving the photogenerated holes. To address this challenge, we have constructed a dual-functional S-scheme ZnO/CdIn 2 S 4 heterojunction systerm coupling the H 2 O 2 generation with a value-added benzylamine (BA) oxidation reaction. In this dual-functional photocatalytic system, photogenerated electrons in CdIn 2 S 4 efficiently reduce O 2 to produce H 2 O 2 , while photogenerated holes in ZnO selectively oxidize BA to N-benzylidenebenzylamine. Leveraging the advantages of the S-scheme heterojunction, the optimized ZnO/CdIn 2 S 4 photocatalyst displays an enhanced H 2 O 2 production rate (386 μmol·L −1 ·h −1 ) and BA oxidation fraction (81%) than pure ZnO or CdIn 2 S 4 . Femtosecond transient absorption (fs-TA) spectroscopy confirm the ultrafast S-scheme electron transfer from the ZnO conduction band (CB) to the CdIn 2 S 4 valence band (VB) upon photoexcitation of the ZnO/CdIn 2 S 4 composite. Besides, timely depletion of VB holes in ZnO and CB electrons in CdIn 2 S 4 can accelerate the interfacial electron transfer in the ZnO/CdIn 2 S 4 S-scheme heterojunction. The innovative design of the ZnO/CdIn 2 S 4 S-scheme photocatalyst provides new insights for developing efficient dual-functional heterojunction photocatalytic systems and introduces a novel method for studying S-scheme heterojunctions using fs-TA spectroscopy.

研究领域: 光催化 · 材料科学 · 环境科学
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY · 2024 · IF 11.2

Insight into bay-/end-substituted perylene diimide and its S-scheme heterojunction for enhanced photocatalytic H2O2 production under visible-light irradiation

Bo Zhang,Kang Li,Renfu Li,Shoufeng Wang,Longtian Kang

Here, 1D bis(N-carboxymethyl) peryleneimide (H 2 PDI), 0D 1,6,7,12-tetrachloro-bis(N-carboxymethyl) peryleneimide (4Cl-H 2 PDI), and 2D 4Cl-H 2 PDI/graphene quantum dot (4Cl-H 2 PDI/GQD) nanostructures are synthesized and carefully analyzed. The effect of bay-/end-substitution and S-scheme heterojunction of PDI-based materials as main catalysts on the photocatalytic H 2 O 2 evolution is first studied through the oxygen reduction reaction (ORR). Under the visible-light irradiation (> 420 nm), 4Cl-H 2 PDI and 4Cl-H 2 PDI/GQD as photocatalysts exhibit the ∼7 and ∼16 times H 2 O 2 evolution rate than H 2 PDI (1059.6 vs. 2484.0 vs. 160.0 µM g −1 h −1 ), respectively. The systematical experiments reveal that 4Cl-H 2 PDI and 4Cl-H 2 PDI/GQD should prefer a two-step single-electron ORR process, while H 2 PDI may involve a 4e ‒ water oxidation and one-step 2e ‒ ORR process. Further experiments confirm that the bay-substitution and GQD doping of H 2 PDI can promote the generation, transportation, and separation of photogenerated electrons and holes, and prolong the carrier lifetime. This work provides insight into PDI-based photocatalytic H 2 O 2 production.

研究领域: 材料科学 · 光化学 · 环境科学
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