ACS Sustainable Chemistry & Engineering
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2024
·
IF 7.1
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.
研究领域:
材料科学
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电化学
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DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
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2024
·
IF 4.7
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.
研究领域:
化学工程
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材料科学
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DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2024
·
IF 8.4
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.
研究领域:
材料科学
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能源工程
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Yingying Zhang,Qiang Huang,Ruoting Wang,Xinjie Du,Yu Yu,Zhe Chen
Modulating the coordination environment of single-atom catalysts (SACs) and designing architectures to maximize the exposure of active sites are pivotal strategies for enhancing peroxymonosulfate (PMS) activation. The fabrication of single-atom‑iron catalysts on support with particular coordination is essential but still remains challenge. Herein, we proposed the construction of single-atom‑iron embedded in graphitic carbon nitride nanosheets (SA-Fe@C 3 N 4 ) catalyst. The layer-confined synthesis strategy realized the loading of single-atom irons and ultrathin C 3 N 4 nanosheet formation in the interlayer of layered template RUB-15. XANES analysis corroborated that the isolated iron atoms are coordinated with three nitrogen and one oxygen atoms (Fe-N 3 O 1 ). Notably, the single iron atoms within the SA-Fe@C 3 N 4 matrix serve as the predominant active sites for PMS activation. The catalyst exhibited exceptional activity for the degradation of sulfamethoxazole (SMX), achieving a mass-normalized rate constant ( k Fe ) of 1.54 × 10 5 min −1 mol −1 with high selectivity toward 1 O 2 /•O 2 − .Theoretical calculations revealed that the Fe-N 3 O 1 moiety accelerated the PMS adsorption and reduced energy barriers for the activation of PMS, thus produce key *O intermediate SO 5 •- and form 1 O 2 /•O 2 − with nearly 100% selectivity. This study supplied a simple avenue to fabricate single-atom‑iron on C 3 N 4 with regulated coordination for wastewater treatment.
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高影响因子
ELECTROANALYSIS
·
2018
·Vol. 30
·期 6
·1033-1040
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IF 2.851
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
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神经科学
·
分析化学
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DOI
高影响因子
Inorganic Chemistry Frontiers
·
2017
·Vol. 4
·期 9
·1533-1538
·
IF 4.036
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
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电化学
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DOI
高影响因子
CHEMISTRY OF MATERIALS
·
2014
·
IF 8.535
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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DOI
高影响因子
Food & Function
·
2016
·Vol. 7
·期 11
·4683-4692
·
IF 2.686
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.
研究领域:
药理学
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毒理学
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细胞生物学
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DOI
PubMed
高影响因子
CHINESE JOURNAL OF CHEMISTRY
·
2017
·Vol. 35
·期 7
·1098-1108
·
IF 1.852
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
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纳米技术
·
电化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
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.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
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.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
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.
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高影响因子
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