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Applied Materials Today · 2022 · IF 8.663

Nanozyme catalyzed cascade reaction for enhanced chemodynamic therapy of low-H2O2 tumor

Chao Jiang,Ting He,Qinan Tang,Jin He,Qiaoju Ren,Dong-Yang Zhang,Bhaskar Gurram,Nicholas Thomas Blum,Yunzhi Chen,Peng Huang,Jing Lin

The efficacy of chemodynamic therapy (CDT) is strongly dependent on the hydrogen peroxide (H 2 O 2 ) level of tumor tissues. Nanozyme-mediated glycolysis reaction is considered as a promising way to supply the amount of H 2 O 2 in situ , therefore, the development of nanozyme-based CDT platform is desirable for low-H 2 O 2 tumor treatment. Herein, we developed a hybrid nanozyme (denoted as MMF-Au) composed of ultrasmall gold nanoparticles (Au NPs) and melanin-coated manganese dioxide flowers (MMF) for enhanced CDT of low-level H 2 O 2 tumors under the guidance of magnetic resonance imaging (MRI) and photoacoustic imaging (PAI). The MMF-Au nanozyme could trigger the cascade reaction of glucose oxidation and Fenton-like reaction. First, the ultrasmall Au NPs with glucose oxidase (GOx)-mimic activity could catalyze the oxidation of glucose to generate large amount of H 2 O 2 . Subsequently, the H 2 O 2 was converted into highly toxic hydroxyl radicals (•OH) via a Mn 2+ -mediated Fenton-like reaction, due to the release of Mn 2+ during the decomposition of MMF in tumor acid microenvironment. Meanwhile, the released Mn 2+ could perform T 1 -weighted MRI. Additionally, the MMF-Au could be used for PAI and photothermal therapy (PTT) due to the strong absorption of melanin in the near-infrared (NIR) region. Both in vitro and in vivo experimental results demonstrated that nanozyme catalyzed cascade reaction could achieve better CDT efficacy in tumors with low level of H 2 O 2 . This study provided a promising strategy to construct nanozyme-triggered cascade reaction system against low-level H 2 O 2 tumors.

研究领域: 癌症治疗 · 纳米医学 · 生物医学工程 · 材料科学 · 成像技术
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY · 2019 ·Vol. 412 ·期 4 ·963-972 · IF 3.286

Preparation of palladium/carbon dot composites as efficient peroxidase mimics for H2O2 and glucose assay

Zhuo Shujuan,Fang Jing,Zhu Changqing,Du Jinyan

In this study, palladium/carbon dot composites (Pd-CDs) were fabricated via a facial hydrothermal route using ethanediamine and palladium chloride dihydrate as precursors. The obtained Pd-CDs showed an excellent intrinsic peroxidase-like activity, which could catalyze the oxidization of 3,3′5,5′-tetramethylbenzidine with the assistance of hydrogen peroxide (H 2 O 2 ) and thus resulted in color change, accompanied by an absorption peak which appeared at 652 nm. Such response is H 2 O 2 concentration–dependent and allows for the assay of H 2 O 2 in the range of 0.1 to 30 μM with a limit of detection of 0.03 μM. Simultaneously, by combination of enzymatic oxidation of glucose with glucose oxidase and Pd-CD catalytic reaction, a colorimetric sensing platform was also constructed for glucose detection with high selectivity and sensitivity (limit of detection as low as 0.2 μM). Additionally, the proposed method exhibited capability for determination of glucose in real samples (fruit juice) with satisfactory recovery (98.5–103%), indicating potential application prospects in biochemical analysis.

研究领域: 生物化学 · 分析化学 · 纳米材料科学
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SENSORS AND ACTUATORS B-CHEMICAL · 2016 · IF 4.758

Facile synthesis of iridium nanoparticles with superior peroxidase-like activity for colorimetric determination of H2O2 and xanthine

Malin Cui,Jingdan Zhou,Yuan Zhao,Qijun Song

A facile and efficient method was developed for the preparation of iridium nanoparticles (Ir NPs) with superior peroxidase-like activity. Under the catalytic action of the Ir NPs, the peroxidase substrate 3,3,5,5-tetramathylbenzidine (TMB) can be oxidized by H 2 O 2 to form a blue-colored production oxTMB. Kinetic analysis indicated that the catalytic behavior was in accordance with the typical Michaelis-Menten kinetics and the catalytic reaction followed the ping-pang mechanism. Electron Spin Resonance (ESR) experiment showed that no hydroxyl radical formed in the reaction process. Peroxide substrates with different electron withdrawing ability (benzoyl peroxide, H 2 O 2 and artemisinin) were used to study the catalytic reactions and results indicated that H 2 O 2 can oxidize TMB with much faster rate than artemisinin and slower rate than benzoyl peroxide. These results suggest an electron transfer mechanism was involved in the system of TMB-H 2 O 2 -Ir NPs. By using TMB as the colorimetric substrate, H 2 O 2 can be rapidly determined and the method was extended for the determination of xanthine based on its production of H 2 O 2 in the presence of xanthine oxidase. The prepared Ir NPs exhibit good stability in wide range of pH and temperature. The Ir NPs retained at least 90% of their initial catalytic activity after stored at ambient temperature for three months. The high specificity for H 2 O 2 and the excellent stability of the peroxidase-like Ir NPs showed the great application potential in biotechnology field.

研究领域: 生物化学 · 分析化学 · 纳米材料科学
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FOOD CHEMISTRY · 2021 · IF 7.514

Protective effect of antioxidant peptides from grass carp scale gelatin on the H2O2-mediated oxidative injured HepG2 cells

Yue-ming Hu,Su-zhen Lu,Ya-si Li,Hui Wang,Yan Shi,Lu Zhang,Zong-cai Tu

The protective effect of antioxidant peptides from grass carp scale gelatin on hydrogen peroxide (H 2 O 2 ) - mediated oxidative injured HepG2 cells was investigated, and the protective mechanism as well as peptide structure were studied. Pretreated with grass carp scale gelatin hydrolysates (GSGH) for 24 h significantly increased the survival rates and decreased the apoptosis rates of H 2 O 2 - mediated oxidative injured HepG2 cells. The increase in SOD, CAT and GPX activities, reduce in ROS level and MDA content, and weaken in damage on cell membrane and DNA could be responsible for the protective effect of GSGH on H 2 O 2 -mediated oxidative injured HepG2 cells. Peptide sequences of GSGH were analyzed by LC-ESI-Q-Orbitrap-MS/MS, and results showed that most of them were low molecular weight peptide at 358–986 Da. Synergistic effect existed among antioxidant peptides and contributed to the strong antioxidant activities of GSGH.

研究领域: 生物化学 · 细胞生物学 · 食品科学
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ACS Nano · 2022 · IF 18.027

Engineering Single-Atom Iron Nanozymes with Radiation-Enhanced Self-Cascade Catalysis and Self-Supplied H2O2 for Radio-enzymatic Therapy

Xianyu Zhu,Jiabin Wu,Ruixue Liu,Huandong Xiang,Wenqi Zhang,Qingchao Chang,Shanshan Wang,Rui Jiang,Feng Zhao,Qiqiang Li,Liang Huang,Liang Yan,Yuliang Zhao

Single-atom nanozymes (SAzymes), with individually isolated metal atom as active sites, have shown tremendous potential as enzyme-based drugs for enzymatic therapy. However, using SAzymes in tumor theranostics remains challenging because of deficient enzymatic activity and insufficient endogenous H2O2. We develop an external-field-enhanced catalysis by an atom-level engineered FeN4-centered nanozyme (FeN4-SAzyme) for radio-enzymatic therapy. This FeN4-SAzyme exhibits peroxidase-like activity capable of catalyzing H2O2 into hydroxyl radicals and converting single-site FeII species to FeIII for subsequent glutathione oxidase-like activity. Density functional theory calculations are used to rationalize the origin of the single-site self-cascade enzymatic activity. Importantly, using X-rays can improve the overall single-site cascade enzymatic reaction process via promoting the conversion frequency of FeII/FeIII. As a H2O2 producer, natural glucose oxidase is further decorated onto the surface of FeN4-SAzyme to yield the final construct GOD@FeN4-SAzyme. The resulting GOD@FeN4-SAzyme not only supplies in situ H2O2 to continuously produce highly toxic hydroxyl radicals but also induces the localized deposition of radiation dose, subsequently inducing intensive apoptosis and ferroptosis in vitro. Such a synergistic effect of radiotherapy and self-cascade enzymatic therapy allows for improved tumor growth inhibition with minimal side effects in vivo. Collectively, this work demonstrates the introduction of external fields to enhance enzyme-like performance of nanozymes without changing their properties and highlights a robust therapeutic capable of self-supplying H2O2 and amplifying self-cascade reactions to address the limitations of enzymatic treatment.

研究领域: 生物医学工程 · 肿瘤学 · 纳米医学
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JOURNAL OF NANOBIOTECHNOLOGY · 2022 ·Vol. 20 ·期 1 ·1-18 · IF 9.429

H2O2-responsive VEGF/NGF gene co-delivery nano-system achieves stable vascularization in ischemic hindlimbs

Chen Youlu,Chen Zuoguan,Duan Jianwei,Gui Liang,Li Huiyang,Liang Xiaoyu,Tian Xinxin,Liu Kaijing,Li Yongjun,Yang Jing

Peripheral vascular disease (PVD) is a common clinical manifestation of atherosclerosis. Vascular endothelial growth factor (VEGF) gene therapy is a promising approach for PVD treatment. However, due to single-gene therapy limitations and high H2O2 pathological microenvironment, VEGF gene therapy are not as expectations and its clinical application are limited. Synergistic effects of Nerve factors and vascular factors in angiogenesis have attracted attention in recent years. In this study, VEGF and nerve growth factor (NGF) genes co-delivery nanoparticles (VEGF/NGF-NPs) were prepared by using H2O2 responsive 6s-PLGA-Po-PEG as a carrier. 6s-PLGA-Po-PEG could react with H2O2 specifically due to the internal peroxalate bond. Angiogenic effects of VEGF/NGF-NPs has been evaluated in cells and hindlimb ischemia mice model. Results showed that VEGF/NGF-NPs promoted VEGF and NGF co-expression simultaneously, eliminated excessive H2O2, strengthened reactions between SH-SY5Ys and HUVECs, and finally enhanced migration, tube formation, proliferation and H2O2 damage resistance of HUVECs. VEGF/NGF-NPs also recovered blood perfusion, promoted the expression of VEGF, NGF, eNOS and NO, and enhanced vascular coverage of pericytes. Treatment effects of VEGF/NGF-NPs may related to VEGF/eNOS/NO pathway. Altogether, VEGF/NGF-NPs eliminated excessive H2O2 while achieving gene co-delivery, and promoted stable angiogenesis. It’s a promising way for PVD treatment by using VEGF/NGF-NPs.Graphical Abstract

CAS / MDL: 38215-36-0 9009-65-8
研究领域: 生物医学工程 · 分子生物学 · 基因治疗 · 血管医学
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CHINESE JOURNAL OF CATALYSIS · 2021 · IF 8.271

Preparation of MIL-88B(Fex,Co1−x) catalysts and their application in one-step liquid-phase methanol oxidation to methyl formate using H2O2

Jianfang Liu,Zhenzhen Ran,Qiyan Cao,Shengfu Ji

The selective oxidation of methanol to methyl formate is one of the most attractive processes to obtain value-added methanol-downstream products. The development of highly efficient and stable catalysts is critical for this transformation. In this study, a series of MIL-88B(Fe x ,Co 1– x ) bimetallic catalysts with different Fe/Co molar ratios were prepared through a one-pot hydrothermal method. X-ray diffraction, scanning electron microscopy, high-resolution transmission electron microscopy, energy dispersive spectroscopy, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, N 2 adsorption-desorption, and inductively coupled plasma-mass spectrometry characterization were performed to elucidate the structure of the catalysts. The activity of the catalysts were assessed in the one-step oxidation of methanol to methyl formate with H 2 O 2 in a liquid-phase batch reactor. The results show that the MIL-88B(Fe x ,Co 1– x ) catalysts exhibit uniform needle-like morphologies with an average length and width of 400–600 nm and 100–150 nm, respectively. Co 2+ is incorporated into the framework by partially replacing Fe 3+ in MIL-88B. Moreover, the catalyst efficiently promoted the conversion of methanol to methyl formate. When MIL-88B(Fe 0.7 ,Co 0.3 ) catalyst was used with a molar ratio of H 2 O 2 to methanol of 0.5 at 80 °C for 60 min, 34.8% methanol conversion was achieved, and the selectivity toward methyl formate was 67.6%. The catalysts also showed great stability with a steady conversion and selectivity even after four cycles. The preliminary oxidation mechanism was also studied. It was determined that H 2 O 2 is first adsorbed on the Fe 3+ sites and subsequently activates these sites. Methanol is adsorbed by the O atoms of the framework through hydrogen bonding and is gradually oxidized to formic acid . Subsequently, formic acid reacts with the residual methanol at the Fe 3+ and Co 2+ Lewis acid sites to form methyl formate.

研究领域: 化学工程 · 催化化学
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Inorganic Chemistry Frontiers · 2022 ·Vol. 9 ·期 16 ·4030-4040 · IF 7.779

c-Axis-penetrated mesoporous MWW zeolite nanosheets: preparation by H2O2-induced micro-explosion and their enhanced properties

Chunna Zhang,Feng Lin,Lingtao Kong,Zhaoqi Ye,Di Pan,Hongbin Li,He Li,Peng Liu,Yahong Zhang,Hongbin Zhang,Yi Tang

Zeolite nanosheets are a burgeoning class of two-dimensional (2D) nanomaterials due to their fascinating properties and diverse applications. However, the effective and controllable preparation of advanced 2D zeolite materials with hierarchical structure and enhanced properties still needs to be investigated. Here, we report highly dispersed oligolayer MWW nanosheets (ca. 2–4 layers) with c-axis-penetrated mesopores, prepared by H2O2-induced micro-explosion coupled with ethanolamine pre-treatment from the multilayered precursor MCM-22P. The vertically aligned mesopores are well merged with intrinsic microporosity within MWW oligolayers with structural integrity. Meanwhile, the removal of OSDA and surface-grafted ethanolamine can be simultaneously achieved apart from the construction of the hierarchical structure. The porosity can be easily regulated by adjusting the H2O2 content, while the framework structure, composition, and intrinsic acidity are retained. Furthermore, benefiting from the greatly improved accessibility of intralayer 10-MR sinusoidal channels, the c-axis-penetrated mesoporous MWW zeolite nanosheet shows enhanced adsorption/diffusion properties and catalytic performances for bulky substrate conversion. This work provides a synergetic post-treatment method for the more rational and controllable design and application of novel layered hierarchical zeolite catalysts, and the efficient and versatile approach reported here shows great potential for industrial applications.

研究领域: 材料科学 · 催化化学
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NEW JOURNAL OF CHEMISTRY · 2022 ·Vol. 46 ·期 25 ·12372-12380 · IF 3.925

A series of novel Cu-based MOFs: syntheses, structural diversity, catalytic properties and mimic peroxidase activity for colorimetric detection of H2O2

Juan Chai,Luohao Yuan,Shiwei Wang,Tong Li,Mingxue Wu,Zhiwei Huang,Hongfeng Yin

Three metal–organic frameworks {[Cu6(L1)4(DMF)(H2O)2·5H2O]}n (1), {Cu3(L1)2(phen)2(H2O)}n (2) and {[Cu8(μ3-OH)3(L2)4(NO3)(H2O)5]·3H2O}n (3) utilizing nitrogen-containing heterocyclic carboxylate bifunctional ligands (L1 = 5-(4-carboxypyridin-3-yl)isophthalic acid and L2 = 2-(5-carboxypyridin-2-yl)terephthalic acid) were self-assembled hydrothermally and characterized. MOFs 1–3 possess 3D networks which consist of three different types of Cu clusters {Cu2O2(OCO)4}, {Cu2O2N4(OCO)2} and {Cu4O10(OCO)4}, respectively. MOFs 1–3 efficiently catalyze the oxidation of cycloalkanes under mild conditions. Besides, the synthesized MOFs 1–3 exhibited high peroxidase-like activity and could be utilized to catalyze the oxidation of 2,2′-azino-bis(3-ethylbenzothiazoline-6-sulphonic acid ammonium salt) (ABTS) to produce green color in the presence of hydrogen peroxide (H2O2). The steady-state kinetics experiments of the oxidation of ABTS catalyzed by MOFs 1–3 were carried out, and the kinetic parameters were obtained. The results indicated that the affinity of MOFs 1–3 towards H2O2 and ABTS was higher than that of the natural horseradish peroxidase (HRP). The as-prepared MOF 1 can be applied for the colorimetric detection of H2O2 with a wide linear range of 0.5 to 200 μM and a limit of detection (LOD) of 0.097 μM. Therefore, the novel Cu-MOFs could be regarded as promising artificial enzyme mimics in catalysis, sensors and environment analysis.

研究领域: 材料科学 · 生物化学 · 分析化学
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Chemosensors · 2022 ·Vol. 10 ·期 6 ·222 · IF 4.229

Differential Sensing of Antibiotics Using Metal Ions and Gold Nanoclusters Based on TMB–H2O2 System

Suqin Liu,Jinjie Wang,Yue Hu,Yunjing Shi,Jingxia Yang,Min Zhang

In the water system, antibiotic pollution significantly impacts the human body and the environment. Therefore, it is essential to quickly identify the types of antibiotics in the system and detect their concentration. It has been reported that many metal ions interact with antibiotics, and some of them can also change the enzyme-like catalytic properties of gold clusters (AuNCs). In the experiments, we found significant differences in the experimental results when different antibiotics and metal ions were placed in a TMB-H2O2system with AuNCs as catalysts. Based on this result, we devised a simple and sensitive colorimetric method for the simultaneous detection of multiple antibiotics using AuNCs-metal ions as the sensor, a multifunctional microplate detector as the detection instrument, and LDA as the analytical method. This method was successfully applied for the identification of antibiotics and the detection of their concentrations in river water.Keywords:gold nanocluster;antibiotic;colorimetric detection;linear discriminant analysis;multiplex detection

研究领域: 环境科学 · 分析化学 · 纳米技术 · 生物技术
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JOURNAL OF ALLOYS AND COMPOUNDS · 2022 · IF 6.371

Facile synthesis of porous 1,3,5-Trihydroxybenzene substituted g-C3N4 for boosted photocatalytic Rhodamine B degradation and H2O2 production

Min Zhang,Yiguo Jiang,Xiuquan Xu,Xiaofeng Yu,Wenyan Shen,Miaomiao Luo,Luyao Ding,Haiwen Chen

The reinforced light-harvesting capability, suppressed photocarrier recombination and increased specific surface area represented a possibility of excellent photocatalytic performance for graphitic carbon nitride (g-C 3 N 4 )-based photocatalysts . Herein, the porous 1,3,5-Trihydroxybenzene substituted g-C 3 N 4 (denoted as PTBCN) composites with superior visible-light-driven photocatalytic properties were rationally constructed via a two-step reaction combination of freeze-drying and thermal-polymerization. The optimal PTBCN-2 achieved the maximum photocatalytic Rhodamine B (Rh B) degradation and H 2 O 2 evolution rate constants, nearly 6.56 and 3.17 times higher than that of bare g-C 3 N 4 . The outstanding performances of PTBCN-2 were probably attributed to the extended specific surface area, robust visible light response, adjusted electronic band structure , accelerated separation and transfer of photocarriers as well as good hydrophilicity. As a result, the above integrated merits were directly responsible for the huge superoxide anion ( • O 2 − ) generation, which dominated the efficient photocatalytic reactions. This work provided a new idea to design and construct high efficiency porous aromatic ring substituted g-C 3 N 4 -related photocatalysts for organic pollutants degradation and H 2 O 2 production.

CAS / MDL: 57-13-6 108-73-6
研究领域: 材料科学 · 环境科学
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Nanomedicine · 2019 · IF 4.717

H2O2/near-infrared light-responsive nanotheronostics for MRI-guided synergistic chemo/photothermal cancer therapy

Yiming Yu,Li Zhang,Miao Wang,Zhe Yang,Leping Lin,Yuxuan Xiong,Zushun Xu,Jing Wang

Aim: To develop a H2O2/near-infrared (NIR) laser light-responsive nanoplatform (manganese-doped Prussian blue@polypyrrole [MnPB@PPy]) for synergistic chemo/photothermal cancer theranostics. Materials & methods: Doxorubicin (DOX) was loaded onto the surface of polypyrrole shells. The in vitro and in vivo MRI performance and anticancer effects of these nanoparticles (NPs) were evaluated. Results: The MnPB@PPy NPs could not only generate heat under NIR laser irradiation for cancer photothermal therapy but also act as an excellent MRI contrast agent. The loaded DOX could be triggered to release by both NIR light and H2O2 to enhance synergistic therapeutic efficacy. The antitumor effects were confirmed by in vitro cellular cytotoxicity assays and in vivo treatment in a xenograft tumor model. Conclusion: The designed H2O2/NIR light-responsive MnPB@PPy-DOX NPs hold great potential for future biomedical applications.

CAS / MDL: 67-68-5 10025-77-1
研究领域: 生物医学工程 · 癌症研究 · 纳米技术 · 医学影像
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