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ELECTROANALYSIS · 2018 ·Vol. 30 ·期 6 ·1033-1040 · IF 2.851

Online Electrochemical Monitoring of Glucose in Rat Brain with Acanthosphere-like CuOOH Nanospheres-based Electrochemical Sensor as Non-enzymatic and O2-independent Detector

Bo Li,Yongzhao Fan,Changqing Li,Xu Zhao,Kun Liu,Yuqing Lin

This study for the first time establishes a reliable non-enzymatic online electrochemical system (OECS) for selective and continuous measuring glucose in animal cerebral system. We proposed a one-step electrochemical method to synthetize a Cu nanostructure directly onto electrode, and over-oxidize it in NaOH to form acanthosphere-like CuOOH nanospheres (denoted as AN-CuOOH), which can serve as an excellent electrochemical catalyst for glucose oxidation and thus for simple and reproducible non-enzymatic glucose detection in strong alkaline solution. To validate the AN-CuOOH-based sensors for in vivo applications, we connect the sensors to a merged solution of in vivo microdialysis and 0.4 M NaOH to set up an OECS for in vivo glucose monitoring in rat brain. The response of this system has strong tolerance to the oxygen and pH fluctuation which may happen in the cerebral brain system during some physiological and pathological processes. The fabricated non-enzymatic OECS has a good linear current response to glucose within a concentration range from 10 to 1000 μΜ with sensitivity of 130.22 nA ⋅ μΜ −1 cm −2 . Additionally, the OECS is stable and does not suffer from the interference coexisting in the cerebral system. With the fabricated non-enzymatic OECS for glucose measurement, the basal level of glucose in the microdialysate from rats striatum was determined to be 248.63 μΜ (n=3). Furthermore, the glucose was clearly decreased to 26.37 % of the basal level when the rat was undergone by 20 min ischemia, and the glucose concentration was gradually restored to 99.15 % during 40 min of reperfusion. Our work propose a technically simple strategy for the fabrication of a highly reproducible non-enzymatic OECS system free from oxygen and pH interference, which is promising in exploring the molecular mechanism associated with brain functions.

研究领域: 生物医学工程 · 神经科学 · 分析化学
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

A bifunctional MnxCo3-xO4-decorated separator for efficient Li-LiI-O2 batteries: A novel strategy to promote redox coupling and inhibit redox shuttling

Dan Li,Ziye Kang,Hao Sun,Ying Wang,Haiming Xie,Jia Liu,Jiefang Zhu

Although redox mediator (RM) strategy can decrease the overpotential in Li-O 2 batteries by tuning the electrochemical formation/degradation of Li 2 O 2 from the circumscribed surface pathway to the solution one, the redox shuttling causes an unexpected RM degradation and a continuous deterioration of Li anode, finally leading to a poor cyclability. This work presents the first report detailing the development of a novel Mn x Co 3-x O 4 -decorated separator for Li-LiI-O 2 batteries. Benefiting from the promotion effect of Mn x Co 3-x O 4 nanocages on I − /I 3 − and I 3 − /I 2 redox coupling, the cell with as-prepared separator maintains a low charge potential of ~3.3 V till the death of cell cycling. In addition, as-prepared separator can efficiently restrain the redox shuttling, leading to an obvious improvement on cycling stability for the cell. Moreover, the contributions of LiI to the battery performance and the operation mechanism are systematically investigated. These results present a promising progress in the development of multi-functional separator materials for RM-involved Li-O 2 batteries and the new design of hybrid energy storage device.

研究领域: 材料科学 · 电化学 · 能源存储技术
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Tailoring the three-phase microenvironment surface to induce carbon nitride oxide generating ·O2– with 100% selectivity for ultrafast photodegradation tetracycline under visible light

Xingyu Zhan,Yunxiong Zeng,Jingcai Xu,Yingchun Xia,Xinqing Wang,Fang Tao,Jie Ouyang,Hongliang Li,Liming Yang,Shenglian Luo,Bo Hong

The reactive oxygen species (ROS) contribute to photodegrading tetracycline (TC), which determines the overall efficiency of photocatalysts. Superoxide radical (·O 2 – ) is one of the excellent ROS for photodegrading TC by carbon nitride. However, achieving hierarchical carbon nitride with efficient, stabile, and selective production of ·O 2 – via O 2 photoreduction is a great challenge. Herein, a carbon nitride oxide nest (CNON 6 ) with carbon/nitrogen vacancies (C-v, N-v) and oxygen substitution (O-s) was prepared via tailoring surface microenvironment. The CNON 6 can photodegrade 82% of TC within 2 min under visible light, and the pseudo-first-order kinetic constant is 1.22 min −1 , 24-fold higher than that of CN. The superior photoactivity is attributed to a unique surface microenvironment, which N-v increased photoelectric conversion efficiency, C-v enhanced O 2 adsorption and O-s induced ·O 2 – evolution with ∼ 100% selectivity. Moreover, PVDF membrane-supported CNON 6 (11.33 cm 2 , 0.88 mg/cm 2 ) can completely remove TC from wastewater at a rate of 2.62 mg/h in a simulated industrial continuous flow cell. The cost-effectiveness assessment was $6.36/kg/h, implying the CNON 6 /PVDF has a bright application prospect in wastewater treatment. This work developed a surface microenvironment tailor strategy to design photocatalysts for efficient degradation of TC.

CAS / MDL: 57-13-6 298-83-9 64-75-5
研究领域: 环境科学 · 材料科学 · 化学工程 · 光催化
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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.

研究领域: 材料科学 · 电化学
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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.

研究领域: 材料科学 · 化学
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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
研究领域: 药理学 · 毒理学 · 细胞生物学
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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.

研究领域: 生物化学 · 纳米技术 · 电化学
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Mixed-ligand metal–organic frameworks with coordinatively un-saturated Co(II) and Ni(II) sites for regenerable O2-selective ad-sorption over N2

Hanbang Liu,Liping Yang,Danhua Yuan,Guangye Liu,Jiacheng Xing,Yunpeng Xu,Zhongmin Liu

For air separation, the separation method relying on adsorbents has attracted wide attention as a low energy consumption process, and the development of O 2 -selective adsorbents is of great significance. Metal-organic frameworks with coordinatively unsaturated transition metal sites have great potential in O 2 -selective adsorption, but most of them cannot be completely regenerated at ambient temperature or can only be effective at very low temperatures. Herein, we report two mixed-ligand metal–organic framework adsorbents [M(AIP)(BPY) 0.5 ·H 2 O] n ·2nH 2 O with coordinatively unsaturated cobalt(II) and nickel(II) sites, which can preferentially adsorb O 2 versus N 2 , and their IAST O 2 /N 2 selectivities are both significantly greater than 1 at 25 °C. These materials exhibited excellent stability and had no loss of adsorption capacities even after immersion in water for 7 days. More importantly, O 2 adsorption–desorption cycle experiments showed that these adsorbents can be completely regenerated at ambient temperature after adsorbing O 2 , and the breakthrough experiments further confirmed their dynamic O 2 /N 2 separation potential and regeneration ability. The results of theoretical calculations suggested that the interactions between adsorbents and O 2 are stronger than those of N 2 , and they have relatively obvious differences in the N 2 and O 2 interaction energies. This work provides inspirations for searching for metal–organic frameworks that can selectively adsorb O 2 at ambient temperature.

研究领域: 材料科学 · 化学工程
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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

Decomposition mechanism of Cl-VOCs on Cu- and Fe-modified activated carbon in an O2-free atmosphere: The oxidation pathway and product distribution

Yuran Li,Zhicheng Xu,Jian Wang,Bin Wang,Tingyu Zhu

Activated carbon exhibits a high adsorption capacity for chlorinated volatile organic compounds (Cl-VOCs), while the desorption of Cl-VOCs is not desirable in the thermal regeneration progress of activated carbon. Chlorobenzene was selected as the model substance to explore whether Cl-VOCs can be oxidized as expected in the regeneration atmosphere of O 2 -free at the temperature range of 150–450 °C. The modification of activated carbon by Cu or Fe has been shown to considerably improve the decomposition activities. According to the breakthrough curves and detection results from XPS and in situ DRIFTS, the decomposition mechanism of C 6 H 5 Cl on Cu and Fe active sites is illustrated. The adsorbed C 6 H 5 Cl is firstly dechlorinated to form C 6 H 6 and *Cl, and then it was found there are two pathways for the C 6 H 6 oxidation. C 6 H 6 is indirectly oxidized to form C 6 H 5 OH and benzoquinone species, or directly ring-opened to generate ethylene and 1,3-butadiene, and further oxidized to produce CO 2 , CO and H 2 O. The C 6 H 6 oxidation is determined by the decomposition of acetate on Cu/AC, but the decomposition of benzoquinone and maleate on Fe/AC. The Fe 3 O 4 and Fe 2 O 3 active sites have a higher dechlorination activity but accelerate the deposition of FeCl 2 , FeCl 3 and organic Cl-containing components. The CuO active center has a higher oxidation performance with a higher CO 2 selectivity. About 83.0–83.5% of adsorbed chlorobenzene has been oxidized, and the main Cl-containing product is HCl accounting for approximately 77.8–81.0%, a small amount of Cl forms polychlorinated organic compounds or metal chlorides occupying 2.0–5.7%. As the regeneration temperature decreases, the total amount of Cl-containing species is reduced due the lower oxidation and dechlorination activity of catalysts. The decomposition products of Cl-VOCs in the thermal regeneration process of activated carbon were clarified and quantified, which provides a theoretical basis to control Cl-VOCs in regeneration gas.

CAS / MDL: 10031-43-3 7782-61-8
研究领域: 环境科学 · 材料科学
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MOLECULES · 2024 ·Vol. 29 ·期 5 ·1094 · IF 4.2

Zn-Doped MnCO3/CS Composite Photocatalyst for Visible-Light-Driven Decomposition of Organic Pollutants

Hui Liang,Yongxin Zhao,Tongjin Liu,Ruijuan Li,Rumei Li,Yuxiao Zhu,Feng Fang

Zn-doped MnCO3/carbon sphere (Zn-doped MnCO3/CS) composites were synthesized using a simple hydrothermal procedure. Among various samples (ZM-50, ZM-05, and ZMC-0), the ternary Zn-doped MnCO3/CS (ZMC-2) catalyst demonstrated excellent visible light-induced photocatalytic activity. This improvement comes from the Zn addition and the conductive CS, which facilitate electron movement and charge transport. The catalyst exhibited efficient degradation of methylene blue (MB) over a wide pH range, achieving a removal efficiency of 99.6% under visible light. Radical trapping experiments suggested that •OH and •O2−played essential roles in the mechanism of organic pollutant degradation. Moreover, the catalyst maintained good degradation performance after five cycles. This study offers valuable perspectives into the fabrication of carbon-based composites with promising photocatalytic activity.

CAS / MDL: 573-58-0 569-64-2
研究领域: 材料科学 · 环境科学 · 化学
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CHEMOSPHERE · 2021 · IF 7.086

Well-dispersed iron and nitrogen co-doped hollow carbon microsphere anchoring by g-C3N4 for efficient peroxymonosulfate activation

Likun Chen,Kewen Xing,Qikai Shentu,Yifei Huang,Weiyang Lv,Yuyuan Yao

Developing single-atom Fenton-like catalysts with the maximum utilization of active sites present an attractive potential in environmental remediation. Herein, the single-atom Fe and N co-doped hollow carbon microsphere loaded g-C 3 N 4 catalyst (HFeNC-g-C 3 N 4 ) was prepared by an innovative cascade anchoring strategy using polystyrene as the hard template, iron phthalocyanine, polydopamine and urea as the Fe, N and C precursor, in which the in-situ generated g-C 3 N 4 could not only effectively anchor Fe atom to create the well-dispersed Fe-N x active sites, but also accelerate the electron transfer in peroxymonosulfate (PMS) activation. Taking advantages of such sequential protecting strategy, the as-synthesized HFeNC-g-C 3 N 4 catalyst with single-atom Fe-N x active sites, verified by XRD , XPS and HAADF-STEM, could work as an efficient Fenton-like catalyst for PMS activation, which achieved almost 100% removal of 4-chlorophenol (4-CP) in 5 min with the turnover frequency calculated to be 34.6 times higher than that of the homogeneous Fe 2+ catalyst. The mechanism of O 2 •- dominated radical combined with nonradical 1 O 2 pathway was confirmed by quenching experiments and ESR analysis, which might be interrelated to the improvement of pH adaptability and interference immunity of HFeNC-g-C 3 N 4 /PMS system. Overall, the present findings provided an innovation strategy for the synthesis of excellent single-atom Fe based catalyst in wastewater purification.

研究领域: 环境科学 · 催化 · 材料科学
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Journal of Environmental Chemical Engineering · 2020 · IF 4.3

Photochemical degradation of chloramphenicol over jarosite/oxalate system: Performance and mechanism investigation

Xuqian Wang,Yi Xie,Wenhua Tong,Wanrong Hu,Yabo Wang,Yongkui Zhang

Rational selection of affordable catalyst and effective degradation process are significant for antibiotic-containing wastewater treatment. Herein, a photochemical catalytic system comprising of bio-synthesized jarosite and oxalic acid (Ox) was investigated for degradation of antibiotic chloramphenicol (CAP) under light irradiation. Benefiting from abundant reactive species including H 2 O 2 , OH, O 2 − produced in photochemical process, a 97.5 % removal efficiency of CAP was obtained within 40 min. Consecutive testing cycles indicated jarosite had excellent stability and reusability in photocatalytic system. Radical chain reaction induced by photosensitive Fe(III)-Ox complexes under light irradiation was suggested to be the main mechanism for CAP degradation. A few degradation intermediates were identified to propose the possible degradation pathways of CAP. Further investigation showed that the antibacterial activities of CAP solution towards Escherichia. coli ATCC 8739 and Staphylococcus. aureus ATCC 6538 were largely reduced after treatment by photochemical process. Typical operation parameters of light/jarosite/Ox system were also investigated. CAP degradation performance in actual water demonstrated the feasibility of light/jarosite/Ox process. Overall, the developed light/jarosite/Ox system possesses great potential for antibiotic-containing wastewater treatment.

CAS / MDL: 56-75-7
研究领域: 环境科学 · 化学工程 · 水处理
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