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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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
·
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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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
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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高影响因子
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
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jiayu Xiao,Luo Hai,Ke Yang,Yuze Luo,Zefeng Wang,Junqin Li,Chunlei Ou,Li Wang,Le Deng,Dinggeng He
Reactive oxygen species (ROS) such as hydroxyl radicals ( OH) and singlet oxygen ( 1 O 2 ) have emerged as promising therapeutic agents for combating biofilm-associated bacterial infections. However, the hypoxic microenvironments in the biofilms severely hinder the ROS production. Herein, we have rationally integrated copper peroxide (CP) and indocyanine green (ICG) into a polydopamine (PDA) nanoparticle to construct a versatile hybrid nanoplatform (PDA/CP/ICG), which can enhance ROS generation for highly efficient biofilm elimination by relieving hypoxic microenvironment. When the PDA/CP/ICG accumulates at the infection site or biofilm, the acidic microenvironment triggers the co-release of Cu 2+ and H 2 O 2 , and the former can catalyze the conversion of self-supplied H 2 O 2 into OH via a Fenton-like reaction and consume the overexpressed antioxidant glutathione (GSH) to further promote the oxidative stress. Moreover, with the help of an 808 nm laser, the hyperpyrexia caused by PDA induces the decomposition of CP into O 2 that is immediately converted by ICG into 1 O 2 . The PDA/CP/ICG shows satisfactory antibacterial and antibiofilm effect due to the self-amplified production of OH and 1 O 2 , and outstanding wound healing with good in vivo biosafety. Overall, this study provides a facile paradigm in ROS-based biofilm elimination, and the proposed hypoxia-irrelevant bactericidal nanoplatform has great potential for future biomedical applications.
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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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ACS Applied Materials & Interfaces
·
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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高影响因子
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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