CHEMICAL ENGINEERING JOURNAL
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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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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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PubMed
高影响因子
SmartMat
·
2022
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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
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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
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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
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2020
·Vol. 34
·期 8
·e4852
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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
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2019
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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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JOURNAL OF POWER SOURCES
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2017
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IF 6.395
Jingbo Yang,Hongwei Mi,Shan Luo,Yongliang Li,Peixin Zhang,Libo Deng,Lingna Sun,Xiangzhong Ren
Flexible Li-O 2 batteries have attracted worldwide research interests and been considered to be potential alternatives for the next-generation flexible devices. Nitrogen-doped carbon nanofibers (N-CNFs) prepared by electrospinning are used as flexible substrate and an amorphous TiO 2 layer is coated by atomic layer deposition (ALD) and then decorated with Ru nanoparticles . The Ru/N-CNFs@TiO 2 composite is directly used as a free-standing electrode for Li-O 2 batteries and the electrode delivers a high specific capacity, improved round-trip efficiency and good cycling ability. The superior electrochemical performance can be attributed to the amorphous TiO 2 protecting layer and superior catalytic activity of Ru nanoparticles. Based on density functional theory (DFT) calculations from first principles, the carbon electrode after coating with TiO 2 is more stable during discharge/charge process. The analysis of Li 2 O 2 on three different interfaces (Li 2 O 2 /N-CNFs, Li 2 O 2 /TiO 2 , and Li 2 O 2 /Ru) indicates that the electron transport capacity was higher on Ru and TiO 2 compared with N-CNFs, therefore, Li 2 O 2 could be formed and decomposed more easily on the Ru/N-CNFs@TiO 2 cathode. This work paves a way to develop the free-standing cathode materials for the future development of high-performance flexible energy storage systems .
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CERAMICS INTERNATIONAL
·
2025
·
IF 5.6
Jun-Min Zhang,Xiao-Wu Chen,Xiao You,Qing-Gang Li,Meng-Meng Wang,Xiang-Yu Zhang,Yan-Mei Kan,Yu-Dong Xue,Shao-Ming Dong
The effect of RE 2 O 3 (RE = La, Y, Er, Lu) on the oxidation behavior of RMI-SiC ceramics in air and wet oxygen atmospheres at 1400 °C were studied. The outward migration of RE 3+ cations reduces the oxidation resistance of SiC-RE ceramics in air, but improves the wet-oxidation resistance of SiC-RE ceramics due to the formation of denser RE 2 Si 2 O 7 layer. The outward migration rates of RE 3+ cations may be influenced jointly by the RE 3+ cation radius and the formation rate of RE 2 Si 2 O 7 . The higher mobility of Er 3+ and Y 3+ cations makes Y 2 O 3 and Er 2 O 3 promising modifier for enhancing the wet-oxidation resistance of RMI-SiC f /SiC composites, although the modified components need to be optimized and further analyzed in a more realistic service environment.
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RESEARCH ON CHEMICAL INTERMEDIATES
·
2024
·
IF 2.8
Yan Jiaqi,Chen Gui,Lu Sihang,Wang Pin,Hu Zhengwu,Chen Wenkai,Yuan Ye
In this work, a stable bimetallic hydrotalcite-derived NiCu/MgAlO catalyst and O 2 as oxidant were used for the toluene oxidation to produce the valuable benzyl alcohol (PhCH 2 OH) and benzaldehyde (PhCHO) under solvent-free and additive-free conditions. This strategy gave 7.2% toluene conversion with 70.7% selectivity to PhCH 2 OH & PhCHO. Multiple characterizations showed that highly dispersed metallic Cu and Ni were anchored on the support surface and a chemical bonding interaction occurred between the metallic Ni and the MgAlO. The metal–support interaction contributed to the formation of active Ni 0 species and NiCu alloy with abundant oxygen defects, resulting in excellent catalytic activity and acceptable stability. A plausible reaction mechanism for the catalytic oxidation of toluene over NiCu/MgAlO catalyst has been proposed. The attractive feature of the present catalytic oxidation system compared to conventional methods was its ability to achieve high selectivity for the desired target product. The further advantage of NiCu/MgAlO catalyzed toluene oxidation was that the reaction temperature and time could be below 180 °C and 2 h, thereby minimizing energy consumption and reducing effluent wastewater, which has potential application prospects.
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高影响因子
VACUUM
·
2023
·
IF 4
Chaoqun Yan,Zhiliang Cheng,Xuan Zhang,Juan Wei,Qian Xu
The photocatalytic efficiency of hematite (α-Fe 2 O 3 ) is limited by its photoexcited state lifetime and diffusion length. By adjusting the surface structure, the photogenerated electron pairs can migrate to the surface and the charge recombination can be suppressed, which can effectively solve these problems and improve the photo-Fenton performance. In this study, four kinds different morphologies of α-Fe 2 O 3 - x (truncated hexagonal bipyramidal, cubic, hexagonal shape, and spherical) were synthesized by hydrothermal method , and a photocatalyst (H-α-Fe 2 O 3 - x ) with higher catalytic activity was prepared by hydrogenation. The results of UV–Vis DRS , PL , Raman, and XPS analysis , the oxygen vacancies and Fe (II) species were introduced into the α-Fe 2 O 3 catalyst after the hydrogenation reaction. The H-α-Fe 2 O 3 - x showed good degradation performance for TC and DX as EMPs model pollutants. The results show that the formation of oxygen vacancy and Fe 2+ is the main factor to improve the photocatalytic activity of the reaction system. Furthermore, the reaction mechanism revealed that reactive radicals involved in the H-α-Fe 2 O 3 - x photocatalytic system were •OH, •O 2 − , and h + responsible. This study provides an alternative technology for an easy and effective means for bandgap engineering to improve the photocatalytic performance of photocatalysts and facilitate widening environmental application.
研究领域:
环境科学
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材料科学
·
化学
·
光催化
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高影响因子
ChemistrySelect
·
2025
·Vol. 10
·期 43
·e04409
·
IF 2
Jialong Yang,Guangqun Zhai
The effect of aerobic dioxygen (O 2 ) residues and hydrogen peroxide (H 2 O 2 ) on dithiobenzoate-mediated reversible addition-fragmentation chain transfer (RAFT) polymerization of methyl methacrylate (MMA) was studied. 2-cyano-2-propyl dithiobenzoate (CPDB) displayed excellent thermally oxidative stability against O 2 in O 2 -rarefied dimethylsulfoxide (DMSO) but was readily oxidized by H 2 O 2 . Azo-initiated CPDB-mediated RAFT polymerization of MMA in DMSO under different media led to multi-component products, consisting of PMMA macro-CTAs, MMA-terminated oligomers and low-MW byproducts, while nitrogen deoxygenating and headspace eliminating gave rise to a comparable CTA efficiency, higher than that headspace limiting. H 2 O 2 -initiated CPDB-mediated headspace-free RAFT polymerization of MMA smoothly proceeded in DMSO even at 50 °C, suggesting the co-initiation by CPDB, and also formed predominant PMMA macro-CTAs, negligible oligomers and some low-MW byproducts. H 2 O 2 -initiated CPDB-mediated headspace-free RAFT polymerization of MMA at 70 °C displayed well-controlled behaviors with 2–5 wt.% byproducts, and the high fidelity of the PMMA macro-CTAs was confirmed by the chain extension via azo-initiated RAFT polymerization and Cu I -catalyzed concurrent ATRP/RAFT polymerization. Graphical AIBN-initiated dithiobenzoate-mediated RAFT polymerization of MMA in O 2 -rarefied DMSO under headspace-free media led to well-controlled behaviors comparable to that under N 2 deoxygenating. H 2 O 2 -initiated RAFT polymerization manifested the unprecedented acceleration by dithiobenzoate; ascribed to its oxidation by H 2 O 2 ; and well-controlled polymerization behaviors.
研究领域:
高分子化学
·
自由基聚合
·
可控/活性聚合
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有机合成
·
材料科学
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危险品化学品经营许可证（带存储）