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Inorganic Chemistry Frontiers · 2017 ·Vol. 4 ·期 9 ·1533-1538 · IF 4.036

Zeolitic imidazole framework derived composites of nitrogen-doped porous carbon and reduced graphene oxide as high-efficiency cathode catalysts for Li–O2 batteries

Ming Zhong,Xin Zhang,Dong-Hui Yang,Bei Zhao,Zhaojun Xie,Zhen Zhou,Xian-He Bu

In this work, a composite of 3D network nitrogen-doped porous carbon on reduced graphene oxide (denoted as NPC/rGO) was derived from pyrolysis of zeolitic imidazolate framework-8 and graphene oxide. The as-prepared NPC/rGO possesses high specific surface area, nitrogen doping and mesopores. When evaluated as the cathode catalyst for Li–O2 batteries, NPC/rGO exhibited higher specific capacity, better cyclability, and greater rate capability than either nitrogen doped porous carbon or reduced graphene oxide. The outstanding performances suggest that zeolitic imidazolate framework derived nitrogen doped porous carbon materials are promising for Li–O2 batteries.

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Food & Function · 2016 ·Vol. 7 ·期 11 ·4683-4692 · IF 2.686

Genistein promotes the metabolic transformation of acetaminophen to glucuronic acid in human L-O2, HepG2 and Hep3b cells via the Nrf2/Keap1 pathway

Fan Yuan-jing,Wei Wei,Luo Jian-ping,Jin Yu-xia,Dai Zi-ling

This study aimed to explore the effects of genistein on regulating the activation of UGTs via the Nrf2/Keap1 pathway and to elucidate the underlying mechanisms of detoxification and hepatic protection. Experiments monitoring genistein-induced protection against acetaminophen-induced cell damage were performed in L-02, HepG2 and Hep3b cells. The results of the MTT, AST, ALT, LDH, GSH and GSSG assays showed that genistein evidently protected the cells from acetaminophen-induced injury in a dose-dependent manner. The control cells were treated with 10 mM acetaminophen without genistein to compare with the effects of the combination of acetaminophen and genistein on the expression of UGT1A1, 1A6 and 1A9, Nrf2 and Keap1 mRNAs, as well as the expression of Nrf2 and Keap1 proteins, which were tested by western blotting. The results showed that the expression of the Nrf2 mRNA and protein increased; in contrast, the expression levels of the Keap1 mRNA and protein were obviously reduced by genistein in a dose-dependent manner. Meanwhile, the expression of the UGT mRNA was increased, and UGT1A9 exhibited the highest expression among the three UGTs. Accordingly, the residual acetaminophen content was obviously reduced and acetaminophen glucuronidation increased after 24 hours of treatment with genistein in a dose-dependent manner.

CAS / MDL: 103-90-2
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CHEMISTRY OF MATERIALS · 2014 · IF 8.535

5-fold Twinned Nanowires and Single Twinned Right Bipyramids of Pd: Utilizing Small Organic Molecules To Tune the Etching Degree of O2/Halides

Na Lu,Wei Chen,Guoyong Fang,Bi Chen,Keqin Yang,Yun Yang,Zhencai Wang,Shaoming Huang,Yadong Li

We report that 5-fold twinned nanowires and single twinned right bipyramids of Pd with high yields can be selectively synthesized in a hydrophilic system with the assistance of acetonitrile and ethanol, respectively. The controlled synthesis is based on an idea that small organic molecules (SOMs) that can attract halide ions via electrostatic interactions of different strengths could well adjust their activity to tune the etching degree of O2/halides for protecting the twinned Pd crystal nucleus. We consider that relatively stronger interaction between acetonitrile and halide ions for the formation of nanowires is due to the existence of three C–Hδ+ bonds induced by the electron-withdrawing CN group of CH3CN, which is confirmed by an as-called iodine starch test, 1H nuclear magnetic resonance spectra, and theoretical calculations. On the basis of this finding, we then have successfully expanded SOMs to other molecules, including acetone, 1,4-dioxane, and 1,3,5-trioxane, which have a function similar to that of acetonitrile for the production of Pd nanowires, and 2-propanol, which has a function similar to that of ethanol for the fabrication of right bipyramids. Although nanowires and bipyramids are both mainly bound by {001} planes, nanowires show better catalytic performance toward the reduction of 4-nitrophenol, indicating that more twin boundaries could offer more active catalytic sites. This work not only provides new information to decrease the degree of etching of O2/halides for controlling twin structure of noble metals but also supports the idea that creating a twin structure is good for enhancing catalytic activity.

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CHINESE JOURNAL OF CHEMISTRY · 2017 ·Vol. 35 ·期 7 ·1098-1108 · IF 1.852

Preparation of Close-Packed Silver Nanoparticles on Graphene to Improve the Enzyme Immobilization and Electron Transfer at Electrode in Glucose/O2 Biofuel Cell

Fengjin Qu,Xiaoyan Ma,Yuchen Hui,Fang Chen,Yan Gao

In this study, chemical reduced graphene-silver nanoparticles hybrid (AgNPs@CR-GO) with close-packed AgNPs structure was used as a conductive matrix to adsorb enzyme and facilitate the electron transfer between immobilized enzyme and electrode. A facile route to prepare AgNPs@CR-GO was designed involving in β -cyclodextrin ( β -CD) as reducing and stabilizing agent. The morphologies of AgNPs were regulated and controlled by various experimental factors. To fabricate the bioelectrode, AgNPs@CR-GO was modified on glassy carbon electrode followed by immobilization of glucose oxidase (GOx) or laccase. It was demonstrated by electrochemical testing that the electrode with close-packed AgNPs provided high GOx loading ( Γ =4.80 × 10 −10 mol•cm −2 ) and fast electron transfer rate ( k s =5.76 s −1 ). By employing GOx based-electrode as anode and laccase based-electrode as cathode, the assembled enzymatic biofuel cell exhibited a maximum power density of 77.437 μW•cm −2 and an open-circuit voltage of 0.705 V.

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JOURNAL OF MEMBRANE SCIENCE · 2024 · IF 8.4

Highly-conductive proton exchange membrane of sulfonated poly(biphenyl alkylene) copolymers for H2/O2 fuel cell with 2.62 W cm-2 power density

Huiting Lin,Yichang Ma,Xiaocan Wang,Guiqin Yi,Aimei Zhu,Qinglin Liu,Qiugen Zhang

Ether-free proton exchange membranes (PEMs) based on aromatic polymers are considered as potential alternatives to perfluorosulfonic acid (PFSA) PEMs due to their low cost, less reactant crossing, exceptional chemical stability and outstanding thermal stability. Herein, a series of high-performance sulfonated poly(biphenyl alkylene) (BPSA-PT- x ) membranes with full carbon chain backbones were synthesized to investigate the effect of different ratios of hydrophobic components on membrane properties. Among the prepared membranes, the BPSA-PT-10 % PEM with the highest proton conductivity (311 mS cm -1 at 80 °C water) possessed excellent dimensional stability (in-plane swelling rate ≤19.7 %, through-plane swelling rate ≤24.9 %), mechanical properties (elongation at break: 89.8 % in wet state), thermal stability (glass transition temperature >450 °C) and low H 2 crossover (1.80 mA cm -2 ). Further, the assembled H 2 /O 2 fuel cell based on BPSA-PT-10 % PEM exhibited competitive performance with a peak power density of 2.62 W cm -2 . The developed poly(biphenyl alkylene)-based PEMs should have potential applications in hydrogen energy field.

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ACS Sustainable Chemistry & Engineering · 2024 · IF 7.1

High Charging Voltage Stable and Air Atmosphere Stable Li–O2 Batteries with an Electrolyte Based on Succinonitrile and In Situ Artificial SEI Construction

Zining Man,Hao Tian,Xingbao Zhu,Zhe Lü

One experiment in this study utilized the plasticizer succinonitrile and lithium salt LiTFSI to directly create an ionic liquid electrolyte, with an artificial solid electrolyte interface layer generated using fluoroethylene carbonate. The typical electrolyte exhibited an ionic conductivity of 10–3 S cm–1 at room temperature and an electrochemical window of up to 5.3 V based on electrochemical impedance spectroscopy and linear sweep voltammetry tests. This electrolyte system effectively addresses the issues of decomposition and deterioration of traditional organic electrolytes in Li–O2 batteries at high voltages (over 4.5 V), as well as the problem of direct oxidation of the anode caused by oxygen shuttling, thereby greatly improving the lifespan of Li–O2 batteries. Additionally, the electrolyte’s low volatility and flame retardancy allowed for reliable operation of the battery in an air atmosphere. A Li–O2 battery assembled with the novel electrolyte was capable of cycling in a pure oxygen atmosphere for more than 1000 cycles at a capacity density of 200 mA h g–1 and over 150 cycles at 500 mA h g–1. Even when connected to ambient air without an additional oxygen selective membrane (OSM), the battery can still cycle continuously for more than 350 and 150 cycles at these two kinds of capacity density.

CAS / MDL: 90076-65-6 114435-02-8
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APPLIED CATALYSIS A-GENERAL · 2024 · IF 4.7

Insight into the synergistic effect between plasma and oxygen vacancy in direct oxidation of CH4 to CH3OH by molecular O2 at mild condition

Kai Li,Junqi Cai,Yue Tao,Yunhe Xing,Zuchao Zhu,Zhiqiang Lu,Xuming Zhang

The direct conversion of methane into the value-added chemical methanol using molecular oxygen was investigated via plasma catalysis under mild condition. An efficient synergistic effect between plasma and catalyst was achieved using an oxygen vacancy-rich ZnO/Al 2 O 3 catalyst. A high methanol selectivity of 48.5 % and a high synergy factor of 2.1 could be achieved simultaneously over ZnO/Al 2 O 3 R300 catalyst. The presence of oxygen vacancies played a crucial role in methanol formation. A close relationship between oxygen vacancy content and methanol selectivity was established. In situ DRIFT and optical emission spectra were employed to identify key intermediates, and a plausible reaction mechanism was proposed. The CH 3 and CH 3 O species were the key intermediates on the catalyst surface. The oxygen vacancy could efficiently adsorb the O radicals and accelerate the formation of CH 3 O species. This work offers insights into the rational engineering of efficient catalyst for plasma catalysis process.

CAS / MDL: 10196-18-6
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ENVIRONMENTAL SCIENCE & TECHNOLOGY · 2022 · IF 11.357

Generation of Reactive Oxygen Species and Degradation of Pollutants in the Fe2+/O2/Tripolyphosphate System: Regulated by the Concentration Ratio of Fe2+ and Tripolyphosphate

Chengwu Zhang,Chuipeng Kong,Paul G. Tratnyek,Chuanyu Qin

Tripolyphosphate (TPP) has many advantages as a ligand for the optimization of the Fe2+/O2 system in environmental remediation applications. However, the relationship between remediation performance and the Fe2+/TPP ratio in the system has not been previously described. In this study, we report that the degradation mechanism of p-nitrophenol (PNP) in Fe2+/O2 systems is regulated by the Fe2+/TPP ratio under neutral conditions. The results showed that although PNP was effectively degraded at different Fe2+/TPP ratios, the results of specific reactive oxygen species (ROS) scavenging experiments and the determination of PNP degradation products showed that the mechanism of PNP degradation varies with the Fe2+/TPP ratio. When CFe2+ ≥ CTPP, the initially formed O2•– is converted to •OH and the •OH degrades PNP by oxidation. However, when CFe2+ < CTPP, the O2•– persists long enough to degrade PNP by reduction. Density functional theory (DFT) calculations revealed that the main reactive species of Fe2+ in the system include [Fe(TPP)(H2O)3]− and [Fe(TPP)2]4–, whose content in the solution is the key to achieve system regulation. Consequently, by controlling the Fe2+/TPP ratio in the solution, the degradation pathways of PNP can be selected. Our study proposed a new strategy to regulate the oxidation/reduction removal of pollutants by simply varying the Fe2+/TPP ratio of the Fe2+/O2 system.

研究领域: 环境科学 · 化学工程 · 材料科学 · 计算化学
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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Fenton-like degradation of sulfamerazine at nearly neutral pH using Fe-Cu-CNTs and Al0-CNTs for in-situ generation of H2O2/OH/O2−

Yong Chen,Zhao Yang,Yunbo Liu,Yong Liu

In this paper, a novel Fenton-like system was constructed by a new catalyst (CNTs-Fe-Cu) combined with Al 0 -CNTs to in situ generate H 2 O 2 from activating O 2 for the degradation of sulfamerazine (SMR). The CNTs-Fe-Cu composite was prepared and characterized by XRD, SEM, EDS and BET methods. The results showed that H 2 O 2 could be generated in-situ by Al 0 -CNTs composite under oxygen aeration, which was then converted to OH and O 2 − radical by CNTs-Fe-Cu composite. The high removal efficiency of SMR could be obtained in Al 0 -CNTs/CNTs-Fe-Cu/O 2 system at a relatively broad range of pH. Furthermore, the removal efficiency of SMR and total organic carbon (TOC) was 85% and 60%, respectively under the following condition: initial pH = 5.8, T = 25 °C, O 2 flow rate = 400 mL/min, CNTs-Fe-Cu = 1 g/L, Al 0 -CNTs = 1 g/L, SMR = 50 mg/L, reaction time = 60 min. In addition, the intermediate products of SMR degradation were identified and the possible degradation pathways of SMR and the degradation mechanism of Al 0 -CNTs/CNTs-Fe-Cu/O 2 process were tentatively proposed.

研究领域: 环境科学 · 化学工程
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JOURNAL OF POWER SOURCES · 2020 · IF 8.247

In-situ grown vanadium nitride coated with thin layer of nitrogen-doped carbon as a highly durable binder-free cathode for Li–O2 batteries

Kailing Sun,Mingrui Liu,Siyan Yu,Huiyu Song,Jianhuang Zeng,Xiuhua Li,Shijun Liao

The Li–O 2 battery is one of the most promising next-generation energy storage systems due to its super-high theoretical energy density . However, its further development is impeded by the current cathode system, which exhibits low energy efficiency and poor cycling stability. Herein, we report a composite of vanadium nitride coated with nitrogen-doped carbon nanoribbons grown in situ on carbon paper (denoted as VN@C) as a novel binder-free cathode for Li–O 2 batteries. We find that the nitrogen-doped carbon coating can significantly improve the stability of VN and enhance the composite's ORR/OER activities. The Li–O 2 batteries with our optimal VN@C-850 cathodes achieve an initial discharge capacity of 8269 mA h g −1 , a discharge-charge voltage gap of 0.88 V, and considerable cycling stability for 183 cycles with a cut-off capacity of 1000 mA h g −1 , compared with 2027 mA h g −1 , 1.21 V, and 12 cycles with uncoated VN cathodes.

研究领域: 电化学 · 能源材料 · 纳米材料 · 电化学储能 · 先进电池技术
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JOURNAL OF CATALYSIS · 2026 · IF 6

Synergistic enhancement of photocatalytic H2O2 production via promoting O2 adsorption and sequential energy/electron transfer process in anthraquinone-engineering of fluorinated metal–organic framework

Shiyi Li,Jie Zhang,Bei Liu,Wanchao Hu,Changli Lü

Solar-driven photocatalytic H 2 O 2 production presents a sustainable alternative to the industrial anthraquinone process. An in situ anthraquinone (AQ) functionalized metal–organic framework (UiO-66-F 4 ) with fluorinated linkers enables efficient concurrent synthesis of H 2 O 2 and value-added benzaldehyde (BzH) in a two-phase system. The AQ-modified F-MOF achieves exceptional H 2 O 2 production rates of 118.1mmol g -1 h −1 under visible light and 328.2mmol g -1 h −1 under simulated sunlight, along with high BzH selectivity (∼95%). Fluorinated linkers and AQ act synergistically to enhance the built-in electric field, promote charge separation, and facilitate oxygen adsorption and activation. RDE and RRDE studies verify a highly selective two-electron oxygen reduction pathway (94% H 2 O 2 selectivity) and reveal a non-traditional mechanism involving energy transfer to form electrophilic 1 O 2 , which is subsequently reduced to •O 2 – by electron and protonated to H 2 O 2 . Both experimental and theoretical results demonstrate that the 1 O 2 mediated pathway proceeds with a lower free energy barrier compared to the molecular oxygen route. Meanwhile, the incorporation of AQ reduces the oxygen adsorption energy and provides additional adsorption sites, further enhancing photocatalytic H 2 O 2 production. EPR spectroscopy corroborates the interconversion between 1 O 2 and •O 2 – during the reaction. This work offers mechanistic insight into the coexistence and interconversion of reactive oxygen species, while demonstrating spontaneous separation and collection of both H 2 O 2 and high-value oxidation products in a two-phase system.

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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Biomimetic O2 Self-generated hybrid membrane nanoplatform for blocking the polarization towards immunosuppressive M2 macrophage phenotype and enhancing sonodynamics therapy in orthotopic colorectal cancer

Ruo-Yun Zhang,Kai Cheng,Xing Sun,Xiao-Quan Yang,Yong Li,Yong-Guo Hu,Xiao-Shuai Zhang,Bo Liu,Wei Chen,Yuan-Di Zhao,Dong-Sheng Huang

Colorectal cancer is one of the most common intestinal tumors, of which occurrence and development are closely related to immune escape activity in vivo . Then, how to comprehensively block immune escape remains a big challenge for immunotherapy. Thus, a biomimetic nanoprobe [email protected] /hybrid membrane/PA ( [email protected] ) is designed by coating Ce6 loaded ZIF-8 with a hybrid membrane composed of neutrophil membrane (Nm) & red blood cell membrane (Rm), accompanied by palmitoyl ascorbate (PA) to achieve reprogramming of immunosuppressive tumor microenvironment (TME) and enhancement of sonodynamics therapy (SDT) in hypoxic tumor. Cell and animal experiments indicate that, the [email protected] probe can specifically target tumor at the inflammatory site, and it can effectively reduce the adsorption of neutrophils, then inhibit the polarization toward immunosuppressive M2 macrophage phenotype. Immunofluorescence staining and ELISA experiments demonstrate that PA and Rm can generate O 2 and significantly improve the hypoxic environment, it enhances the polarization of anti-tumor M1 macrophages and regulate related cytokines, meanwhile improves the therapeutic effect of SDT. The survival rate of mice is elevated to 100% within 60 d. Overall, this O 2 self-generated biomimetic hybrid membrane nanoprobe can block immune escape from various aspects and obtain enhanced SDT effect, then increase the treatment efficiency of inflammatory tumor, significantly improve the prognosis and elevate the survival rate of mice, providing a new idea for the clinical diagnosis and treatment of colitis-associated tumors.

研究领域: 癌症研究 · 纳米技术 · 免疫治疗 · 生物医学工程
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