APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Hongwei Zhu,Xu Yin,Yi Wang,Kajia Wei,Liankai Gu,Yonghao Zhang,Zhenshan Duan,Zhen Huang,Haoming Chen,Weiqing Han
This study developed a self-supported MOF/FeOOH heterojunction cathode without binders for boosted Fe(Ⅲ) reduction in heterogeneous electro-Fenton (EF) processes. The electron transport channels from FeOOH to in-situ grown NH 2 -MIL-88B(Fe) were established through the spontaneous formation of an internal electric field (IEF), which enhanced the electrical conductivity and disrupted the chemical inertness of the Fe(Ⅲ) reduction. The MOF/FeOOH cathode increased sulfamethazine (SMT) removal up to 95.76 %, 2.5 times better than using PTFE as binders. After ten-consecutive degradation experiments, the Fe(Ⅱ) content at cathode surface increased from 39.23 % to 56.73 %. Density functional theory (DFT) calculations and advanced characterization techniques demonstrated the efficient Fe(Ⅲ) reduction and H 2 O 2 activation during the reaction. These results elucidate the promoting effect of modulating the “contact” between the catalyst and current collectors, as to provide a feasible and promising strategy for the development of efficient heterogeneous EF cathodes.
研究领域:
环境科学
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材料科学
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电化学
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催化
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产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2019
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IF 7.149
Zhihao Chen,Xuchun Li,Shujuan Zhang,Jiyuan Jin,Xiaojie Song,Xiaomeng Wang,Paul G. Tratnyek
Research efforts on advanced oxidation processes (AOPs) have long been focused on the fundamental chemistry of activation processes and free radical reactions. Little attention has been paid to the chemistry of the precursor oxidants. Herein, we found that the precursor oxidants could lead to quite different outcomes. A counterintuitive result was observed in the photoreduction of bromate/iodate: the combination of H2O2 and UV enhanced the reduction of bromate/iodate, whereas the addition of persulfate to the UV system led to an inhibitory effect. Thermodynamic and kinetic evidence suggests that the reduction of bromate in UV/H2O2 was attributable to the direct reaction between HOBr and H2O2. Both experimental determination and kinetic simulation demonstrate that the reaction between HOBr and H2O2 dominated over the •OH-mediated reactions. These results suggest that H2O2 possesses some particular redox properties that distinguish it from other peroxides. The prototypical UV/H2O2 process is not always an AOP: it can also be an enhanced reduction process for chemicals with intermediates that are reducible by H2O2. Considering the increasing interest in persulfate-based AOPs, the results of this study identify some novel advantages of the classical H2O2-based AOPs.
研究领域:
环境化学
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水处理
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化学工程
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DOI
PubMed
高影响因子
TALANTA
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2017
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IF 4.162
Yaoyao Zhou,Bo Ling,Hongqi Chen,Lun Wang
A novel fluorescence method for the determination of hydrogen peroxide (H 2 O 2 ) and uric acid (UA) was developed. The procedure was based on the hydroxyl radicals (·OH), which effectively quenched the fluorescence of the Mn 2+ -doped NaYF 4 :Yb,Er upconversion nanoparticles (UCNPs). Based on the property of Mn 2+ -doped NaYF 4 :Yb,Er upconversion nanoparticles, the Fenton reaction and enzymatic reaction of uric acid, this method could be used for highly sensitive detection of H 2 O 2 and uric acid. Under optimal conditions, we observed that the fluorescence quenching signal showed good linearity with the H 2 O 2 concentration in the range of 3.00 × 10 -8 M ~ 6.00×10 -5 M, and the detection limit of this assay was 1.30×10 -8 M. Meanwhile, the linear concentration range for UA was 4.00 × 10 -9 M ~ 1.00×10 -5 M, and the lower limit of detection was 1.90×10 -9 M. Furthermore, the developed method was successfully used for the determination of UA levels in human serum with satisfactory results.
研究领域:
分析化学
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生物化学
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纳米技术
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产品关联
DOI
PubMed
高影响因子
Science Advances
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2020
·Vol. 6
·期 18
·
IF 13.117
Chen-Cheng Xue,Meng-Huan Li,Yang Zhao,Jun Zhou,Yan Hu,Kai-Yong Cai,Yanli Zhao,Shu-Hong Yu,Zhong Luo
The rapid development of treatment resistance in tumors poses a technological bottleneck in clinical oncology. Ferroptosis is a form of regulated cell death with clinical translational potential, but the efficacy of ferroptosis-inducing agents is susceptible to many endogenous factors when administered alone, for which some cooperating mechanisms are urgently required. Here, we report an amorphous calcium carbonate (ACC)–based nanoassembly for tumor-targeted ferroptosis therapy, in which the totally degradable ACC substrate could synergize with the therapeutic interaction between doxorubicin (DOX) and Fe2+. The nanoplatform was simultaneously modified by dendrimers with metalloproteinase-2 (MMP-2)–sheddable PEG or targeting ligands, which offers the functional balance between circulation longevity and tumor-specific uptake. The therapeutic cargo could be released intracellularly in a self-regulated manner through acidity-triggered degradation of ACC, where DOX could amplify the ferroptosis effects of Fe2+ by producing H2O2. This nanoformulation has demonstrated potent ferroptosis efficacy and may offer clinical promise.
研究领域:
肿瘤学
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纳米技术
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药学
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细胞生物学
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产品关联
DOI
PubMed
高影响因子
TALANTA
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2018
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IF 4.244
Yanli Zhou,Congming Li,Yuanqiang Hao,Baoxian Ye,Maotian Xu
High-density and cross-linked copper-based metal-organic framework (Cu-MOF) sheets were successfully prepared via a simple oriented growth method on a carboxylated graphene-modified electrode surface. Hydrogen peroxide (H 2 O 2 ) was selected as a model molecule to examine the performance of the thin film of Cu-MOF/graphene. The proposed sensor showed an extended linear detection range from 2.00 × 10 −7 to 1.85 × 10 −4 mol L −1 ( R = 0.998), a high sensitivity of 0.792 A (mol L −1 ) −1 , and a low detection limit of 6.7 × 10 −8 mol L −1 , due to the synergistic catalysis from the porous structure and favorable electron transfer mediating function of the electroactive Cu-MOFs and the high conductive property of the graphene. The reduction peak current of H 2 O 2 changed less than 3.7% in the presence of 57-fold high concentrations (2.0 × 10 −4 mol L −1 ) of the potential interfering species. The good selectivity of the prepared modified electrode was acquired by the size exclusion (molecular sieving) for H 2 O 2 because of the proper pore shape and pore size of Cu-MOFs. The feasibility of the assay was verified by test of H 2 O 2 in disinfectant samples. The proposed strategy presents valuable information related to the construction of non-enzymatic electrochemical sensors .
研究领域:
材料科学
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电化学
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分析化学
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传感器
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产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry B
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2018
·Vol. 6
·期 42
·6858-6864
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IF 4.776
Wenying Li,Jiayan Wang,Jiacheng Zhu,Yue-Qing Zheng
Nanomaterial-based artificial enzymes (nanozymes), as an emerging generation of artificial enzymes, have received extensive attention in recent years owing to their striking merits. In this study, the obtained Co3O4 nanocrystals exhibited catalase-like activity and could catalyze the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) in the presence of H2O2, and a clear absorption peak at 652 nm can be observed. It was verified that the catalytic activity for the oxidation of TMB originated from the oxygen, which is generated by Co3O4 catalyzed H2O2 decomposition. Upon addition of glutathione (GSH), the catalytic ability of the Co3O4 nanocrystals was inhibited. And, the changes of absorbance at 652 nm could be utilized to quantify the concentration of GSH. Under the optimized conditions, the proposed assay showed good linear relationships and a low detection limit towards GSH. Moreover, the Co3O4 nanocrystals had excellent stability and can maintain the catalytic activity for a long time. Thus, a simple, sensitive and selective nanozyme-based biosensor was developed for the colorimetric detection of GSH.
研究领域:
纳米技术
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分析化学
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生物化学
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产品关联
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
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2021
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IF 8.198
Chaoping Li,Yibing Pi,Su Liu,Jingwen Feng,Xu Zhang,Shiye Li,Rong Tan
Pickering interfacial catalysis enables oil/water biphasic reactions to efficiently proceed by the formation of stable Pickering emulsions. However, a convenient approach to control the emulsion properties, so as to combine the reactivity and recovery of catalytic emulsifiers, remains challenging to date. Herein, we have reported the switchable transition between emulsification/demulsification controlled by the catalytic reaction process, to realize reaction-controlled Pickering interfacial catalysis. A novel series of phosphotungstate (PW)-functionalized mesoporous Janus silica nanosheets were thus prepared by selectively decorating ammonium PW on one side of mesosilica nanosheets. Characterization results suggested their H2O2-switched reversible emulsification/demulsification behavior in an oil/water biphasic system due to H2O2-induced wettability change in the ammonium PW moiety. The resultant H2O2-switchable Pickering emulsions induced an efficient Pickering interfacial catalysis approach for selective oxidation of alcohols by aqueous H2O2 in water, thus leading to remarkable high conversion and selectivity over a wide range of alcohols. When H2O2 was used up, they could be demulsified spontaneously, resulting in the complete separation of catalytic emulsifiers for steady reuse. The reaction-controlled emulsification/demulsification approach provided a sustainable way to combine reactivity and recovery of catalytic emulsifiers in Pickering interfacial catalysis, which was a benefit for energy-saving in industrial applications.
研究领域:
材料科学
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催化
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纳米技术
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化学工程
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产品关联
DOI
高影响因子
MICROCHIMICA ACTA
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2022
·Vol. 189
·期 7
·1-10
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IF 6.408
Li Haolin,Sun Huiyuan,Ding Jianwei,Wu Ting,Cai Shuangfei,Wang Chen,Yang Rong
The successful synthesis of ruthenium oxide/reduced graphene oxide (RuO 2 /rGO) heterostructures by one-pot hydrothermal method using graphene oxides and RuCl 3 as precursors is reported. The heterostructures had high peroxidase-like (POD-like) activities, which catalyzes the oxidation of classical peroxidase substrate 3,3′,5,5′-tetramethylbenzidine (TMB) in the presence of H 2 O 2 to create a blue colored reaction product. The catalytic activity was significantly enhanced by the synergistic effect between RuO 2 nanoparticles and rGO. RuO 2 /rGO had a low K m of 0.068 mM and a high v max of 1.228 × 10 −7 M·s −1 towards TMB in the TMB-H 2 O 2 catalytic oxidation system. In addition, the POD-like activity originating from the electron transfer mechanism was confirmed by cytochrome C (Cyt C) oxidation experiment. A colorimetric method based on RuO 2 /rGO heterostructures was developed with good sensitivity and selectivity for glucose detection with a limit of detection of 3.34 μM and a linear range of 0–1500 μM. The RuO 2 /rGO heterostructures have potential applications in the biomedical areas, such as biosensor and diagnostics. Graphical abstract
研究领域:
生物传感器
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分析化学
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材料科学
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生物医学工程
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF CONTROLLED RELEASE
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2024
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IF 10.5
Guitao Tan,Chenyang Qi,Qinqin Zhang,Haonan Hu,Bingtian Tu,Jing Tu
Bacterial infection is a major impediment towards wound healing and threaten human health worldwide. Traditional antibiotic therapy poses a high risk of inducing bacterial resistance, thus nanomaterial-based synergistic bactericidal strategy as effective alternatives have received tremendous attention. Herein, a NIR/pH-dual responsive nanoplatform was fabricated for synergistic photothermal and chemodynamic therapy (PTT/CDT). Prussian blue (PB) were employed as supporting material, while copper peroxide (CP) were growth in situ on PB surface, resulting in a core-shell structured nanoplatform (designated as PC). PB core served as photothermal/Fenton catalyst dual agents, and CP shell could co-release Cu 2+ and H 2 O 2 under acidic bacterial infection environment, realizing synergistic PTT and H 2 O 2 -releasing CDT. Under NIR irradiation, PC exhibited photothermal-enhanced Fenton-like reaction feature and the hyperthermia facilitated Cu 2+ release, leading to the rapid conversion of H 2 O 2 into toxic •OH to effectively kill Gram-negative Escherichia coli ( E. coli ) and Gram-positive Staphylococcus aureus ( S. aureus ), eradicating S. aureus biofilm. Moreover, the released Cu 2+ could improve the bactericidal effect of CDT via the depletion of GSH and significantly promote cell migration. Furthermore, in vivo experiments demonstrated PC with good biocompatibility exhibited robust bactericidal effect and promoted wound healing. Overall, this versatile nanoplatform offered an efficacious and safe antibiotic-free strategy for bacterial infection treatments.
研究领域:
纳米技术
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生物医学工程
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材料科学
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微生物学
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治疗学
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产品关联
DOI
PubMed
高影响因子
ACS Applied Nano Materials
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2024
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IF 5.3
Xingxing Jiang,Aomei Zhang,Huan Gou,Xiang Chen,Lei Deng,Minghui Yang
Highly pathogenic bacterial infections are a major threat to human health, and the resulting drug resistance is beginning to pose a major clinical threat. To combat multidrug-resistant bacterial infections, there is an urgent need to develop antimicrobial drugs that are highly effective, environmentally friendly, and able to prevent the emergence of bacterial resistance. In this paper, Co4N nanozymes were successfully synthesized by pyrolysis of a presynthesized Co-containing metal organic framework (Co-MOF). Its peroxide and lactate oxidase activity and antimicrobial properties were investigated. Without the addition of exogenous H2O2, the nanozymes can initially generate H2O2 by catalyzing lactic acid and then produce highly active •OH from H2O2. This approach overcomes the obstacle of insufficient H2O2 to achieve a satisfactory antimicrobial effect. Furthermore, the local high temperature generated by Co4N under 808 nm laser irradiation further enhanced the antibacterial effect. These results showed that the nanozyme possesses broad-spectrum antimicrobial activity against Escherichia coli and Staphylococcus aureus, with an inhibition rate as high as 99% within 2 h. Meanwhile, the enzyme has good biocompatibility, paving a way for the application of MOF materials in biomedical fields.
研究领域:
生物医学
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材料科学
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微生物学
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
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2024
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IF 8.1
Zhicheng Wang,Chen Wang,Xiaohui Wu,Wen-Da Oh,Mingjie Huang,Tao Zhou
Electrochemical advanced oxidation processes (EAOPs) based on natural air diffusion electrode (NADE) promise efficient and affordable advanced oxidation water purification , but the sustainable operation of such reaction systems remains challenging due to severe cathode electrowetting. Herein, a novel floating cathode (FC) composed of a stable hydrophobic three-phase interface was established by designing a flexible catalytic layer of FC. This innovative electrode configuration could effectively prolong the service life of the cathode by mitigating the interference of H 2 bubbles from the hydrogen evolution reaction (HER), and the H 2 O 2 production rate reached 37.59 mg h −1 ·cm −2 and realize a long-term stable operation for 10 h. Additionally, an FC/carbon felt (CF) dual-cathode electro-Fenton system was constructed for in situ sulfamethoxazole (SMX) degradation. Efficient H 2 O 2 production on FC and Fe(III) reduction on CF were synchronously achieved, attaining excellent degradation efficiency for both SMX (ca. 100%) with 2.5 mg L −1 of Fe(Ⅱ) injection. For real wastewater , the COD removal of the FC/CF dual-cathode electro-Fenton system was stabilized at exceeding 75%. The practical application potential of the FC/CF dual-cathode electro-Fenton system was also demonstrated for the treatment of actual landfill leachate in continuous flow mode. This work provides a valuable path for constructing a sustainable dual-cathode electro-Fenton system for actual wastewater treatment .
研究领域:
环境科学
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电化学工程
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水处理技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-13
·
IF 14.7
Wu Yuhan,Zhao Yuying,Yuan Qixin,Sun Hao,Wang Ao,Sun Kang,Waterhouse Geoffrey I. N.,Wang Ziyun,Wu Jingjie,Jiang Jianchun,Fan Mengmeng
Carbon nanomaterials show outstanding promise as electrocatalysts for hydrogen peroxide (H 2 O 2 ) synthesis via the two-electron oxygen reduction reaction. However, carbon-based electrocatalysts that are capable of generating H 2 O 2 at industrial-level current densities (>300 mA cm −2 ) with high selectivity and long-term stability remain to be discovered. Herein, few-layer boron nanosheets are in-situ introduced into a porous carbon matrix, creating a metal-free electrocatalyst (B n -C) with H 2 O 2 production rates of industrial relevance in neutral or alkaline media. B n -C maintained > 95% Faradaic efficiency during a 140-hour test at 300 mA cm −2 and 0.1 V vs. RHE, and delivered a mass activity of 25.1 mol g catalyst −1 h −1 in 1.0 M Na 2 SO 4 using a flow cell. Theoretical simulations and experimental studies demonstrate that the superior catalytic performance originates from B atoms with adsorbed O atoms in the boron nanosheets. B n -C outperforms all metal-based and metal-free carbon catalysts reported to date for H 2 O 2 synthesis at industrial-level current densities.
研究领域:
材料科学
·
电化学
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催化科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）