ChemSusChem
·
2023
·
IF 8.4
Juanjuan Han,Yangyang Zhang,Xiumeng Zheng,Yuyang Lu,Wanting Li,Xiaorong Zhou,Zhandong Ren,Yi Liu,Meixue Hu,Li Xiao,Lin Zhuang
Graphical A novel AEM with good strength and flexibility was synthesized by combining rigid PPO and flexible PVA. Dual cationic groups were added to improve ion concentration and create ion channels, enhancing ion conductivity. Cross-linking and phase separation improved the AEM's resistance to alkali. A series of cross-linked AEMs ( c -DQPPO/PVA) are synthesized by using rigid polyphenylene oxide and flexible poly(vinyl alcohol) as the backbones. Dual cations are grafted on the PPO backbone to improve the ion exchange capacity (IEC), while glutaraldehyde is introduced to enhance compatibility and reduce swelling ratio of AEMs. In addition to the enhanced mechanical properties resulting from the rigid-flexible cross-linked network, c -DQPPO/PVA AEMs also exhibit impressive ionic conductivity, which can be attributed to their high IEC, good hydrophilicity of PVA, and well-defined micro-morphology. Additionally, due to confined dimension behavior and ordered micro-morphology, c -DQPPO/PVA AEMs demonstrate excellent chemical stability. Specifically, c -DQPPO/PVA-7.5 exhibits a wet-state tensile strength of 12.5 MPa and an elongation at break of 53.0 % at 25 °C. Its OH − conductivity and swelling degree at 80 °C are measured to be 125.7 mS cm −1 and 8.2 %, respectively, with an IEC of 3.05 mmol g −1 . After 30 days in a 1 M NaOH solution at 80 °C, c -DQPPO/PVA-7.5 experiences degradation rates of 12.8 % for tensile strength, 27.4 % for elongation at break, 14.7 % for IEC, and 19.2 % for ion conductivity. With its excellent properties, c -DQPPO/PVA-7.5 exhibits a peak power density of 0.751 W cm −2 at 60 °C in an H 2 -O 2 fuel cell.
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高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
·
2021
·
IF 2.495
Qian-Qian Huang
A novel tetranuclear nickel(II)-flavonolate complex [Ni II 4 (fla) 4 (CH 3 O) 4 (H 2 O) 4 ] (flaH: 3-Hydroxyflavone, flavonol) was synthesized. Its crystal structure and spectroscopic features have been investigated in details by physicochemical methods and single crystal X-ray diffraction. Different from other mononuclear metal-flavonolate complexes, this complex demonstrates a cluster molecular structure which has four Ni II centers, and each Ni II centre is coordinated by a bidentate flavonolate, three methanol and a water molecule. The crystal of this complex is tetragonal crystal system: space group I 41/a, a = 24.4361(14), b = 24.4361(14), c = 12.7972 (14), α = β = γ = 90 ° , V = 7641.5 (12), Z = 4. The complex can react with O 2 , in other words, it has enzymatic reactivity just like enzyme-substrate model of quercetin 2,3-dioxygenase, and the reaction products are similar with the other reported enzyme-substrate models.
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Advanced Materials Interfaces
·
2018
·Vol. 5
·期 22
·1801070
·
IF 4.834
Lin Fan,Doudou Lou,Haoan Wu,Xizhi Zhang,Yefei Zhu,Ning Gu,Yu Zhang
In spite of the competitive advantages, inorganic nanoparticle mimic enzymes exhibit inherent disadvantages of limited catalytic efficiency and lacking selectivity. Here, a gold nanoparticle (AuNP)-based mimic enzyme with significantly enhanced glucose selectivity and catalytic activity is constructed and demonstrated for the first time. Aminophenylboronic acid is employed to increase the affinity to glucose, as well as build molecular imprinted polymer shells to realize the selectivity for template molecules of glucose. Besides that, heptadecafluoro- n -octyl bromide nanoemulsion with the function of providing oxygen is introduced to gain a further improvement in catalytic activity, which successfully enhances the catalytic efficiency ( k cat / K m ) up to about 270-fold. Based on the demonstrated catalytic properties, AuNP-based glucose oxidase mimics are successfully applied in practical glucose detection of drinks and blood glucose.
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ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Zhongxi Xie,Shuang Liang,Xuechao Cai,Binbin Ding,Shanshan Huang,Zhiyao Hou,Ping’an Ma,Ziyong Cheng,Jun Lin
Hypoxia and overexpression of glutathione (GSH) are typical characteristics of the tumor microenvironment, which severely hinders cancer treatments. Here, we design a novel biodegradable therapeutic system, O2–Cu/ZIF-8@Ce6/ZIF-8@F127 (OCZCF), to simultaneously achieve GSH depletion and O2-enhanced combination therapy. Notably, the doped Cu2+ doubles the O2 storage capacity of the ZIF-8 matrix, which makes OCZCF an excellent pH-sensitive O2 reservoir for conquering tumor hypoxia, enhancing the photodynamic therapy (PDT) efficiency of chlorin e6 (Ce6) under 650 nm laser irradiation. Moreover, the released Cu2+ can act as a smart reactive oxygen species protector by consuming intracellular GSH. The byproduct Cu+ will undergo highly efficient Fenton-like reaction to achieve chemodynamic therapy (CDT) in the presence of abundant H2O2. The accompanying O2 will further alleviate hypoxia. The in vitro and in vivo experimental data indicate that OCZCF could cause remarkable tumor inhibition through enhanced synergetic PDT and CDT, which may open up a new path for cancer therapy.
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高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2016
·
IF 5.393
Ting Liu,Lucheng Xue,Xin Guo,Jia Liu,Yu Huang,Chuguang Zheng
The reaction mechanisms of a mixture gas of HCl, O2, and SO2 in Hg0 adsorption on α-Fe2O3(001) surface are clarified by a group of adsorption experiments and theoretical calculations based on the density functional theory. The role of O2 in removing Hg0 is greatly influenced by the reaction temperature, meanwhile, the O atom coverage could affect the adsorption performance of Hg0. The dissociated O2 competes with the active sites of Cl species on Fe surface at low temperature, however, at medium temperature HCl and O2 could simultaneously facilitate the Hg0 transformation. Combined with the theoretical calculations, the role of SO2 and the probable pathways in removing Hg0 are discussed. Lower concentration of SO2 as well as HCl could dissociate on α-Fe2O3(001) surface, and the intermediates combine with gaseous Hg0, forming mercury–sulfur, mercury–chlorine compounds, and so forth. In addition, the different concentrations of SO2 are also discussed, and the corresponding X-ray photoelectron spectroscopy analysis on contrasted samples is conducted to research the morphological characterization, providing a reliable basis for judging the probable pathways of Hg0 transformation.
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高影响因子
Small
·
2016
·Vol. 12
·期 39
·5477-5487
·
IF 8.315
Zhifang Ma,Mengchao Zhang,Xiaodan Jia,Jing Bai,Yudi Ruan,Chao Wang,Xuping Sun,Xiue Jiang
Local hypoxia in tumors, as well as the short lifetime and limited action region of 1 O 2 , are undesirable impediments for photodynamic therapy (PDT), leading to a greatly reduced effectiveness. To overcome these adversities, a mitochondria-targeting, H 2 O 2 -activatable, and O 2 -evolving PDT nanoplatform is developed based on Fe III -doped two-dimensional C 3 N 4 nanofusiform for highly selective and efficient cancer treatment. The ultrahigh surface area of 2D nanosheets enhances the photosensitizer (PS) loading capacity and the doping of Fe III leads to peroxidase mimetics with excellent catalytic performance towards H 2 O 2 in cancer cells to generate O 2 . As such tumor hypoxia can be overcome and the PDT efficacy is improved, whilst at the same time endowing the PDT theranostic agent with an effective T 1 -weighted in vivo magnetic resonance imaging (MRI) ability. Conjugation with a mitochondria-targeting agent could further increase the sensitivity of cancer cells to 1 O 2 by enhanced mitochondria dysfunction. In vitro and in vivo anticancer studies demonstrate an outstanding therapeutic effectiveness of the developed PDT agent, leading to almost complete destruction of mouse cervical tumor. This development offers an attractive theranostic agent for in vivo MRI and synergistic photodynamic therapy toward clinical applications.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Leilei Hou,Siyang Yan,Liping Liu,Jiaxu Liu,Guang Xiong
The TS-1 microsphere was facilely prepared via a direct spray drying of the mixture containing the nanocrystal TS-1 and mother liquor. The calcined TS-1 zeolites possess a hollow structure and numerous intercrystalline mesopores, which may facilitate the diffusion properties. Au nanoparticles were loaded on TS-1 support by utilizing a deposition–precipitation process to prepare the Au/TS-1-M catalysts for propylene epoxidation in the presence of H 2 and O 2 conditions. The effects of the Ti and Au loadings on the structure, porosity, morphology, and catalytic performances of the Au/TS-1 catalysts have been investigated by various techniques. Under the optimized synthesis conditions (Si/Ti molar ratio = 57, 0.49 wt% Au), a propylene conversion of 6.1 % and a PO selectivity of 91.7 % were obtained on the Au/TS-1 catalyst. A PO formation rate of 186.8 g PO ·kg cat. −1 ·h −1 was achieved at the 20th hour.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Xueyi Zhang,Wenshuang Sun,Yue Wang,Zhen Li,Xianqiang Huang,Tielong Li,Haitao Wang
In this study, we prepared a micron zero-valent iron/ N -doped graphene-like biochar (mZVI/NGB) composite using a mechanochemical method for tetracycline (TC) degradation through O 2 activation. The mZVI and NGB components formed a strong coupling catalytic system, with mZVI acting as an electron pool and NGB as a catalyst for H 2 O 2 generation. Under circumneutral pH (5.0–6.8), the mZVI/NGB composite exhibited exceptional TC removal efficiency, reaching nearly 100 % under optimal conditions. It also showed good tolerance to co-existing anions, such as Cl - , SO 4 2- , and humic acid. Further studies found that the TC degradation mechanism was mainly ascribed to the non-radical pathway ( 1 O 2 and electron transfer), and the Fe 2+ /Fe 3+ redox cycle on the composite's surface also played a crucial role in maintaining catalytic activity. This research contributes to the development of advanced materials for sustainable and effective water treatment, addressing pharmaceutical pollutant contamination in water sources.
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高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Xichen Sun,Pengfei Wang,Liuyan Tang,Ningning Li,Yan-Ru Lou,Yuezhou Zhang,Peng Li
An effective method capable of simultaneously providing antibacterial activity, blood glucose regulation, and angiogenesis promotion for healing bacteria-infected diabetic wounds is not reported to date, but urgently required. In this study, a hydrogel composite ( γ -PGA/PDA/GOx/WO x (PPGW)), endowed with these desired attributes is fabricated by incorporating polydopamine (PDA), glucose oxidase (GOx), and tungsten oxide (WO x ) nanowires into the poly( γ -glutamic acid) ( γ -PGA) framework. The exceptional photothermal conversion properties of PDA facilitated notable antibacterial effects on bacteria-infected diabetic wounds; GOx regulated high blood glucose by consuming glucose and generating hydrogen peroxide (H 2 O 2 ); while WO x nanowires displayed remarkable photocatalytic abilities, converting H 2 O 2 into oxygen (O 2 ) when exposed to 808-nm near-infrared radiation. Density functional theory calculations and experiments are conducted to confirm the mechanism of WO x -mediated photocatalytic degradation of H 2 O 2 to produce O 2 . These transformations aided in alleviating the hypoxic conditions in wounds associated with diabetes, expediting angiogenesis, and fostering cell crawling and proliferation. Consequently, the multifunctional hydrogel dressing PPGW, featuring photothermal, antibacterial, and enzyme-catalyzed activity reduces hyperglycemia at the wound site. Moreover, photocatalytic O 2 production represents a promising strategy for addressing chronic bacteria-infected diabetic wounds.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Jiahui He,Zhenlong Li,Jueying Chen,Jiaxin Wang,Lipeng Qiao,Baolin Guo,Juan Hu
It is still challenging to design stimuli-responsive smart hydrogel dressing to promote bacteria-infected diabetic wound healing from the whole healing stage by intelligently responding to external stimuli or wound microenvironment. In addition, nitric oxide (NO) and oxygen (O 2 ) have been shown to accelerate diabetic wound healing by promoting angiogenesis and alleviating hypoxia. A series of NIR/glucose stimuli-responsive multifunctional smart hydrogels with NO/O 2 dual gas-releasing properties was designed based on N-carboxyethyl chitosan-grafted-phenylboronic acid (CECP), oxidized dextran (OD), ε-polylysine (EPL)-coated manganese dioxide (EMn), and β-cyclodextrin-reduced graphene oxide/N, N’-di-sec-butyl-N, N’-dinitroso-1,4-phenylenediamine (rGB) via dual dynamic crosslinking to promote bacteria-infected diabetic wound healing. The added rGB and EMn as photothermal agents rapidly kill bacteria through photothermal therapy. Meanwhile, rGB endows CECP/OD/EMn/rGB hydrogels to release NO under NIR stimulation to promote angiogenesis. Nanozyme EMn with catalase (CAT)/superoxide dismutase (SOD)-like activity can scavenge ROS and release O 2 to alleviate hypoxia and oxidative stress. The phenylboronic acid in CECP forming phenylboronate ester structure endows hydrogel with glucose-controlled release of doxycycline. NIR/glucose stimuli-responsive CECP/OD/EMn/rGB hydrogels with NO/O 2 dual gas-releasing property in a full-thickness skin wound-infected diabetic model reduced the inflammation, promoted wound contraction, collagen deposition, angiogenesis, and alleviated wound hypoxia, providing new ideas for treating bacteria-infected diabetic wounds.
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高影响因子
COMBUSTION AND FLAME
·
2018
·
IF 4.494
Guoqing Wang,Yuyang Li,Wenhao Yuan,Yizun Wang,Zhenbiao Zhou,Yingzheng Liu,Jianghuai Cai
Bio-butanol is an important alternative fuel and has many advantages in engine combustion . In the present work, laminar flame propagation of n- butanol/air and n- butanol/(14% O 2 /86% He) mixtures was investigated using a constant-volume combustion vessel at the unburnt temperature of 423 K, initial pressures of 1–20 atm and a series of equivalence ratios. Flame instabilities of n -butanol, including cellular instability and pulsating instability, were studied based on flame morphology. The unsteady transition from weak flame to normal flame was investigated based on the flame trajectories and this phenomenon became less perceptible in the flame with stronger combustion intensity and smaller Lewis number. The accelerated laminar burning velocity (LBV), thickened flame thickness, larger Markstein length and Markstein number indicate that the thermal diffusivity of n- butanol/O 2 /He flames are greatly enhanced by helium addition. The smaller densities and lower reactant concentrations result in the smaller laminar burning fluxes of n- butanol/O 2 /He flames than those of n -butanol/air flames. The high temperature kinetic model of n -butanol reported by Cai et al. was further developed with recent theoretical progresses on n -butanol reactions. The updated high temperature model was validated on the present experimental data and a vast amount of previous n -butanol combustion data . Sensitivity analysis was performed using the updated model under wide pressure and equivalence ratio ranges. The similarity in the sensitivities indicates that the sensitive reactions in n- butanol/air flames can be validated by using n- butanol/O 2 /He flames, which greatly compensates the problem that the n- butanol/air flames are susceptible to flame instabilities at high pressures. The weaker pressure dependence of the LBVs of n -butanol/O 2 /He flames indicates that their flame chemistry changes less to resist the pressure variation.
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Catalysis Science & Technology
·
2024
·
IF 4.4
Renjie Deng,Huajie Liu,Haishuai Cui,Yao Tian,Hai Yang
In this work, we have developed a green method for the preparation of para-nitrotoluene through the catalytic nitration of toluene with nitrogen dioxide (NO2) under the promotion of dioxygen (O2). The experimental results reveal that the dealumination of Hβ zeolite has a significant effect on the catalysis of the developed NO2–O2–acetic anhydride (Ac2O) system, in which the conversion of toluene is 78.1% and the selectivity to para-nitrotoluene is 71.8%. Furthermore, the nature of different dealuminated catalysts was investigated by nitrogen adsorption–desorption analysis, X-ray diffraction (XRD), Fourier-transform infrared (FT-IR), thermal gravimetric analysis (TGA), inductively coupled plasma (ICP), ammonia temperature-programmed desorption (NH3-TPD), pyridine adsorbed Fourier-transform infrared (Py-FT-IR), scanning electron microscopy (SEM) and 27Al magic-angle spinning nuclear magnetic resonance (27Al MAS NMR) techniques. The results of characterization indicate that the structure of the Hβ zeolite still remains and that of Al species in the extra-framework is preferentially removed after acid treatment. Based on the combined results of catalytic characterization and DFT calculation, a feasible reaction mechanism of improved para-selectivity in toluene nitration was suggested for the NO2–O2–Ac2O system.
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