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.
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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.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2022
·
IF 11.357
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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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
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
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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高影响因子
JOURNAL OF CATALYSIS
·
2026
·
IF 6
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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ACS Applied Materials & Interfaces
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2022
·
IF 10.383
Pei-Pei Luo,Xin-Ke Zhou,Yu Li,Tong-Bu Lu
Solar energy-driven direct CH4 conversion to liquid oxygenates provides a promising avenue toward green and sustainable CH4 industry, yet still confronts issues of low selectivity toward single oxygenate and use of noble-metal cocatalysts. Herein, for the first time, we report a defect-engineering strategy that rationally regulates the defective layer over TiO2 for selective aerobic photocatalytic CH4 conversion to HCHO without using noble-metal cocatalysts. (Photo)electrochemical and in situ EPR/Raman spectroscopic measurements reveal that an optimized oxygen-vacancy-rich surface disorder layer with a thickness of 1.37 nm can simultaneously promote the separation and migration of photogenerated charge carriers and enhance the activation of O2 and CH4, respectively, to •OH and •CH3 radicals, thereby synergistically boosting HCHO production in aerobic photocatalytic CH4 conversion. As a result, a HCHO production rate up to 3.16 mmol g–1 h–1 with 81.2% selectivity is achieved, outperforming those of the reported state-of-the-art photocatalytic systems. This work sheds light on the mechanism of O2-participated photocatalytic CH4 conversion on defective metal oxides and expands the application of defect engineering in designing low-cost and efficient photocatalysts.
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SmartMat
·
2022
·
IF 0
Yajun Ding,Yuanchao Huang,Yuejiao Li,Tao Zhang,Zhong-Shuai Wu
The realization of high-efficiency, reversible, stable, and safe Li-O 2 batteries is severely hindered by the large overpotential and side reactions, especially at high rate conditions. Therefore, rational design of cathode catalysts with high activity and stability is crucial to overcome the terrible issues at high current density. Herein, we report a surface engineering strategy to adjust the surface electron structure of boron (B)-doped PtNi nanoalloy on carbon nanotubes (PtNiB@CNTs) as an efficient bifunctional cathodic catalyst for high-rate and long-life Li-O 2 batteries. Notably, the Li-O 2 batteries assembled with as-prepared PtNiB@CNT catalyst exhibit ultrahigh discharge capacity of 20510 mAh/g and extremely low overpotential of 0.48 V at a high current density of 1000 mA/g, both of which outperform the most reported Pt-based catalysts recently. Meanwhile, our Li-O 2 batteries offer excellent rate capability and ultra-long cycling life of up to 210 cycles at 1000 mA/g under a fixed capacity of 1000 mAh/g, which is two times longer than those of Pt@CNTs and PtNi@CNTs. Furthermore, it is revealed that surface engineering of PtNi nanoalloy via B doping can efficiently tailor the electron structure of nanoalloy and optimize the adsorption of oxygen species, consequently delivering excellent Li-O 2 battery performance. Therefore, this strategy of regulating the nanoalloy by doping nonmetallic elements will pave an avenue for the design of high-performance catalysts for metal-oxygen batteries.
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DALTON TRANSACTIONS
·
2021
·Vol. 50
·期 44
·16386-16394
·
IF 4.39
Fozia Sultana,Khaled Althubeiti,Khamael M. Abualnaja,Jiahui Wang,Abid Zaman,Asad Ali,Safeer Ahmad Arbab,Sarir Uddin,Qing Yang
For safety concerns, polymer-based Li–O2 batteries have received more attention than traditional non-aqueous Li–O2 batteries. However, poor cycling stability, low round trip efficiency, and over charge potential during cycling are the major shortcomings for their future applications. In this work, a soluble redox mediator integrated into a polymer electrolyte provides immediate access to the solid discharged product, lowering the energy barrier for reversible Li2O2 generation and disintegration. Moreover, introducing a redox mediator to the polymer electrolyte boosts the ORR during discharge and the OER during the recharge process. The synergistic redox mediator pBQ (1,4 benzoquinone) dramatically reduces the over-potential. A small proportion of pBQ in the polymer electrolyte allows Li2O2 to develop in a thin film-like morphology on the cathode surface, resulting in a high reversible capacity of ∼12 000 mA h g−1 and an extended cycling stability of 100 cycles at 200 mA g−1 with a cut-off capacity of 1000 mA h g−1. The remarkable cell performance is attributed to the fast kinetics of para benzoquinone for the ORR and OER in Li–O2 batteries. The use of a redox mediator in a polymer electrolyte opens a new avenue for practical Li–O2 battery applications in achieving low charge potential and excellent energy efficiency.
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Green Energy & Environment
·
2020
·
IF 6.395
Zhaoning Song,Juncong Yuan,Zhenping Cai,Dong Lin,Xiang Feng,Nan Sheng,Yibin Liu,Xiaobo Chen,Xin Jin,De Chen,Chaohe Yang
The advocacy of green chemical industry has led to the development of highly efficient catalysts for direct gas-phase propene epoxidation with green, sustainable and simple essence. The S-1/TS-1@dendritic-SiO 2 material with three-layer core–shell structure was developed and used as the support for Au catalysts, which showed simultaneously fantastic PO formation rate, PO selectivity and stability (over 100 h) for propene epoxidation with H 2 and O 2 . It is found that silicalite-1 (S-1) core and the middle thin layer of TS-1 offer great mass transfer ability, which could be responsible for the excellent stability. The designed dendritic SiO 2 shell covers part of the acid sites on the external surface of TS-1, inhibiting the side reactions and improving the PO selectivity. Furthermore, three kinds of SiO 2 shell morphologies (i.e., dendritic, net, mesoporous shell) were designed, and relationship between shell morphology and catalytic performance was elucidated. The results in this paper harbour tremendous guiding significance for the design of highly efficient epoxidation catalysts.
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BIOMEDICAL CHROMATOGRAPHY
·
2020
·Vol. 34
·期 8
·e4852
·
IF 1.728
Jing Wang,Yong Zhang,Meiqi Zhou,Meizhu Zheng,Jing Cui,Zhiqiang Liu,Chunming Liu,Shu Liu
Superoxide anion radical scavenger and xanthine oxidase inhibitor play an important role in the treatment of several relevant human diseases. In the present study, ultrafiltration liquid chromatography–mass spectrometry coupled to microplate reader was applied to screen and identify superoxide anion radical scavengers and xanthine oxidase inhibitors from total flavonoids of Ginkgo biloba leaves. As a result, four compounds (quercetin, apigenin, kaempferol and isorhamnetin) were screened as xanthine oxidase inhibitors by ultrafiltration LC–MS, and the 50% scavenging concentration values of the screened flavonoids were lower than those for allopurinol. Lineweaver–Burk plot results indicated that kaempferol was a competitive xanthine oxidase inhibitor; the other flavonoids were all anticompetitive inhibitors. Four flavonoids—rutin, quercetin, kaempferol and isorhamnetin—were screened as superoxide anion radical scavengers by LC–MS. The results demonstrate that the method for screening and evaluation of superoxide anion radical scavenger and xanthine oxidase inhibitor from a complex mixture system is feasible and efficient.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2019
·
IF 5.107
Sharafat Ali,Izaz Ali Shah,Haiou Huang
The need for high-performance and novel technologies for selective treatment of radionuclides in water has recently stimulated broad research. In this study, we examined the ability of carbon nanotube (CNT) membranes in selective removal of strontium (Sr 2+ ) and cesium (Cs + ) from water and wastewater. In single-metal systems that contained only Sr 2+ , Cs + or their competitive metal ions, the distribution coefficients ( K d ) of functionalized CNT membranes for divalent cations, i.e., Sr 2+ , Ca 2+ , and Mg 2+ , were measured as 4.41 mmol g −1 , 2.14 mmol g −1 , and 1.30 mmol g −1 , respectively, and those for monovalent cations, i.e., Cs + , K + and Na + , were 0.81 mmol g −1 , 0.79 mmol g −1 , and 0.81 mmol g −1 , respectively. When Cs + or Sr 2+ co-existed with a competing cation, both pristine and functionalized CNT membranes showed excellent selectivity to Sr 2+ over Mg 2+ and Ca 2+ while their selectivity to Cs + over K + and Na + diminished. Moreover, the CNT membranes remained their selectivity for Sr 2+ in a wastewater effluent despite the complex water composition. Overall, the selectivity sequence of the CNT membranes for divalent cations support the occurrence of inner-sphere complexation on CNT surfaces, while that for the monovalent cations was probably determined by electrostatic interactions. This study demonstrates that Ar/O 2 plasma treatment is a greener technology for the production of CNT functionalized membranes for selective removal of contaminants from water to achieve “fit-for-purpose” treatment.
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