CHEMICAL ENGINEERING JOURNAL
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2026
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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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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
·
IF 11.3
Hao Liu,Siqing Cheng,Jianjun Chen,Xiaoping Chen,Shangchao Xiong,Fang Huang,Houfeng Liu,Junhua Li,Chuanzhi Sun
Mitigating industrial nitrous oxide (N2O) emissions is critical for climate action, yet developing efficient low-temperature N2O decomposition catalysts under O2-containing conditions remains challenging. The weak oxygen–support interaction leads to unsatisfactory N2O decomposition performance in the supported Co3O4/CeO2 catalyst. This study aims to enhance the electronic oxide–support interaction in the Co3O4/CeO2 catalyst through Zn doping, thereby improving its catalytic performance for N2O decomposition under O2-rich conditions. The results demonstrate that, in the presence of 5% O2, the activation energy of the catalyst sharply decreases from 117.5 to 60.4 kJ·mol–1 after Zn doping (Co2.4Zn0.6O4/CeO2). Additionally, the doped catalyst exhibits strong durability to the O2 + H2O + NOx impurity gas components. Advanced spectral characterization and density functional theory calculations reveal that Zn doping modulates the geometry and electronic structure of active cobalt sites, optimizing the adsorption and activation capabilities of N2O molecules. This study elucidates the mechanism of N2O decomposition over the catalysts and establishes a clear structure–activity relationship between the atomic-scale configuration of active sites and their performance. These findings provide critical insights for designing efficient supported oxide catalysts through targeted doping strategies and offer new perspectives for developing highly efficient and low-energy N2O decomposition catalysts.
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高影响因子
APPLIED CATALYSIS A-GENERAL
·
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
·
材料科学
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ACS Sustainable Chemistry & Engineering
·
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
·
电化学
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JOURNAL OF MEMBRANE SCIENCE
·
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
·
能源工程
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CHEMISTRY OF MATERIALS
·
2014
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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
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化学
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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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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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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ELECTROANALYSIS
·
2018
·Vol. 30
·期 6
·1033-1040
·
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.
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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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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
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.
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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.
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