JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2022
·
IF 8.91
Jianzheng Zhen,Shisong Nie,Jiahao Sun,Shiyuan Pan,Jinhui Wang,Jian Sun,Weiyang Lv,Yuyuan Yao
Developing highly efficient and stable catalysts for peroxymonosulfate (PMS) based advanced oxidation processes (AOPs) are crucial in the field of environmental remediation. In this work, a facile encapsulated-precursor pyrolysis strategy was reported to prepare a competent PMS-activation catalyst, in which uniformly distributed Fe 3 O 4 nanoparticles were firmly anchored on porous boron nitride (BN) nanosheets by N-doped carbon shell (NC layer). Taking advantage of strong metal-support interaction, the as-synthesized catalyst (BFA-500) could efficiently activate PMS to achieve 100% removal of 4-chlorophenol (4-CP) in 6 min, and the corresponding turnover frequency (TOF) value was 1–2 orders of magnitude higher than that of the benchmark homogeneous (Fe 2+ ) and nanoparticle (Fe 0 and Fe 3 O 4 ) catalysts. Moreover, the well protected encapsulated structure of BFA-500 ensured the remarkable stability that could effectively resist the interference of complex water environment, including initial pH value, various inorganic ions and actual water, and its catalytic activity remained almost unchanged in 5 use-regeneration cycles. More importantly, the generation of O 2 •- and 1 O 2 radicals for the 4-CP removal in BFA-500/PMS system was ascribed to Fe 3 O 4 boosted C–N sites containing pyridinic N, where electrons transferred from the embedded Fe 3 O 4 nanoparticles to C–N sites to secure the PMS dissociation into reactive radicals. Overall, this work provided a promising way to design desired PMS-activation catalyst toward wastewater purification.
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JOURNAL OF MEDICINAL CHEMISTRY
·
2021
·
IF 7.446
Zhipeng Chen,Lina Zhang,Junjie Yang,Lu Zheng,Fanjie Hu,Siqin Duan,Kutty Selva Nandakumar,Shuwen Liu,Hang Yin,Kui Cheng
The previous virtual screening of ten million compounds yielded two novel nonlipopeptide-like chemotypes as TLR2 agonists. Herein, we present the chemical optimization of our initial hit, 1-phenyl-3-(thiophen-2-yl)urea, which resulted in the identification of SMU-C80 (EC50 = 31.02 ± 1.01 nM) as a TLR2-specific agonist with a 370-fold improvement in bioactivity. Mechanistic studies revealed that SMU-C80, through TLR1/2, recruits the adaptor protein MyD88 and triggers the NF-κB pathway to release cytokines such as TNF-α and IL-1β from human, but not murine, cells. To the best of our knowledge, it is the first species-specific TLR1/2 agonist reported until now. Moreover, SMU-C80 increased the percentage of T, B, and NK cells ex vivo and activated the immune cells, which suppressed cancer cell growth in vitro. In summary, we obtained a highly efficient and specific human TLR1/2 agonist that acts through the MyD88 and NF-κB pathway, facilitating cytokine release and the simultaneous activation of immune cells that in turn affects the apoptosis of cancer cells.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2020
·
IF 4.939
Ting Pan,Baohua Yue,Liuming Yan,Guangbo Zeng,Yidong Hu,Shufa He,Wei Lu,Hongbin Zhao,Jiujun Zhang
Novel functionalized polysulfone with high local density of sulfonic acid groups, N , N -bis(sulfopropyl)aminyl-4-phenyl polysulfone or O , O′ -bis(sulfopropyl)resorcinol-5-yl-4-phenyl polysulfone (PSF-X-C 3 H 6 SO 3 H, X = N or O) are synthesized. These polymers are synthesized by bromination of polysulfone followed by Suzuki cross-coupling reaction to graft the aminophenyl groups and the dimethoxyphenyl groups onto the polymeric backbone, followed by introduction of the sulfopropyl groups via sultone ring-opening reaction. In addition, the composite membrane of PSF-O-C 3 H 6 SO 3 H and PSF-N-C 3 H 6 SO 3 H is also synthesized for comparison. The maximum proton conductivity of composite PSF-O-C 3 H 6 SO 3 H and PSF-N-C 3 H 6 SO 3 H reaches 46.66 mS cm −1 at 95 °C and 90% RH, higher than PSF-O-C 3 H 6 SO 3 H (42.06 mS cm −1 ) and PSF-N-C 3 H 6 SO 3 H (38.76 mS cm −1 ). Meanwhile, the composite exhibits compromised water uptake and swelling ratio, and low methanol permeability . The excellent overall performance of the composite is attributed to phase-separation between the hydrophilic and the hydrophobic subphases, and the hydrogen-bonding network developed in the hydrophilic subphases.
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JOURNAL OF CHEMICAL THERMODYNAMICS
·
2019
·
IF 2.29
Wentian Li,Hu Lin,Nan Song,Gaoquan Chen,Xinbao Li,Hongkun Zhao
Solubilities of gimeracil (form P) in aqueous co-solvent mixtures of isopropanol, N,N -dimethylformamide (DMF), ethylene glycol (EG) and dimethylsulfoxide (DMSO) were investigated via the isothermal dissolution equilibrium method at (283.15–328.15) K under ambient pressure p = 101.2 kPa. Experimental solubility was increased with increasing temperature and mass fraction of each co-solvent. The largest solubility was found in neat co-solvents. The solids equilibrated with liquid phase were characterized by X -ray power diffraction, indicating no polymorphic transformation, solvate formation or crystal transition according to the spectral data. The Jouyban-Acree model was adopted to correlate the obtained solubility. The highest RAD and RMSD values were, respectively, 2.61 × 10 −2 and 14.96 × 10 −4 . Quantitative values for the local mole fraction of DMF (EG, DMSO or isopropanol) and water around gimeracil (form P) were acquired by using the Inverse Kirkwood–Buff integrals method. The preferential solvation parameters for isopropanol were positive in the isopropanol mixtures in intermediate and isopropanol-rich compositions, which indicated that gimeracil (form P) was preferentially solvated by isopropanol. Gimeracil (form P) could act mainly as a Lewis acid interacting with proton-acceptor functional group of isopropanol. Within the same region, gimeracil (form P) was not preferentially solvated by DMF, EG and DMSO. Furthermore, the method of linear solvation energy relationships was performed with a suitable combination of solvent polarity descriptors to explain the nature of intermolecular interactions resulting in the solubility variation in the co-solvent mixtures.
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Advanced Materials Interfaces
·
2018
·Vol. 5
·期 23
·1801149
·
IF 4.834
Shuguang Wang,Jinwen Qin,Lirong Zheng,Donglei Guo,Minhua Cao
Controllable synthesis of 2D carbon nanosheets with high heteroatom-doping level, large specific surface area, and hierarchically pore structure is difficult and desired. In this work, a novel and simple self-sacrificing in situ formed dual-template strategy is first developed to synthesize N/S codoped hierarchically porous carbon nanosheets. The in-situ formed g -C 3 N 4 and amorphous ZnO act as self-sacrificing templates on account of their thermal decomposition and evaporation at higher temperature. The N/S codoped hierarchically porous carbon nanosheets simultaneously possess high heteroatom-doping level (N: 10.51 wt%; S: 1.71 wt%), large specific surface area (904.63 m 2 g −1 ), and abundant hierarchically porous structure. Particularly, this material possesses a high content of pyridinic-N and pyrrolic-N configuration (65.66%). These unique structure advantages of N/S codoped hierarchically porous carbon nanosheets contribute to high oxygen reduction electrocatalytic activity in both basic and acidic environments. Additionally, as the anode material for sodium-ion batteries, the material also displays a high reversible capacity of 270.1 mAh g −1 at a current density of 100 mA g −1 and high stability (160.1 mAh g −1 after 2000 cycles at 1000 mA g −1 with a capacity retention of 82.3%). These results indicate a great potential of the material in energy conversion and storage applications.
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Soft Matter
·
2015
·Vol. 11
·期 14
·2885-2892
·
IF 4.029
Dashuang Fan,Peizhu Zheng,Yuanming Ma,Tianxiang Yin,Jihua Zhao,Weiguo Shen
The concentration-dependent enthalpies of mixing for water/sodium bis(2-ethylhexyl)-sulfosuccinate (AOT)/n-alkane microemulsions with different water contents ω0 and chain lengths n of n-alkane were determined by isothermal titration microcalorimetry (ITC) and flow-mixing microcalorimetry at 298.15 K and used to calculate the interaction enthalpies (−ΔHC) between the droplets. It was found that −ΔHC increased with ω0, and changed from negative to positive at about ω0 = 10. The investigation of the dependence of −ΔHC on n revealed that the values of −ΔHC were negative and had a minimum for ω0 = 5; while they were positive and had a maximum for ω0 = 15. These phenomena were discussed based on the competition of the overlapping contribution of the surfactant tails between two neighbouring droplets and the penetration contribution of the solvent molecules into the surfactant tails. These results indicated the important role of entropy in the stability of the microemulsion systems.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2016
·
IF 4.758
Zongen Liu,Jiecheng Xiao,Xianwei Wu,Liqing Lin,Shaohuang Weng,Min Chen,Xiaohui Cai,Xinhua Lin
This work reports a facile and effective approach for preparing graphene quantum dots co-doped with nitrogen and sulfur (N-S/GQDs). The proposed method comprised pyrolysis of citric acid with glutathione and dialysis treatment. The fabricated N-S/GQDs exhibited blue luminescence and a high fluorescence quantum yield of 36.3%. N-S/GQDs can be sensitively quenched by Fe 3+ , which was absorbed on the edge of N-S/GQDs through the coordination interaction between Fe 3+ and N, S elements. The subsequent introduction of pyrophosphate ion (PPi) resulted in the recovery of the fluorescence of Fe 3+ -quenched N-S/GQDs. The stronger coordination reactivity between Fe 3+ and PPi induced changes in fluorescence. PPi concentration was facilely quantified through the recovered amplitudes of the fluorescence intensities of N-S/GQDs. Under the optimized experimental condition, increased fluorescence intensity showed a linear relationship to PPi concentration (1 μM to 1000 μM) in serum samples. Additionally, the proposed method featured sensitive and selectivity for the detection of PPi in synovial fluid, suggesting the potential application for simple and accurate clinical diagnosis of arthritic diseases.
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2024
·
IF 5.8
Jiajia Ma,Zhiheng Ye,Jie Zhou,Zhong-Ting Hu,Qianqian Wang,Junliang Wang,Zhiyan Pan,Mian Hu
In this study, the influences of soybean straw (SS) to spirulina platensis (SP) mass ratios and pyrolysis temperature on the evolution properties of N-containing species in pyrolytic tri-products and the nitrogen migration mechanism and involved chemical reactions during the co-pyrolysis processes were comprehensively investigated. Results indicated that co-pyrolysis of SS ang SP significantly facilitated the transformation of nitrogen into N bio-oil and N char from N gas . Increasing the amount of SP led to a decrease in the concentration of NH 3 and HCN in N gas , while their concentrations increased gradually with temperature increasing. NH 3 and HCN formation was due to H radicals attacking the N-sites of N-heterocyclic, with NH 3 formation being more strongly influenced by this process. Regarding N char , increasing the ratio of SP enhanced nitrogen incorporation reactions and promoted formation of pyridinic-N and pyrrolic-N. Conversely, decreasing the ratio of SP enhanced hydrogenation and condensation reactions, which favored the formation of quaternary-N. With increasing temperature, protein-N decomposed significantly, while pyridinic-N, pyrrolic-N, and quaternary-N remained stable. Additionally, pyridinic-N can convert to quaternary-N at temperature > 500 °C. Increasing the SP ratio greatly decreased oxygenates content while increased that of N-containing compounds in N bio-oil . The content of heterocycle-N (34.31 %) and nitriles (9.22 %) in bio-oil peaked at a ratio of 1:3, attributed to SP promoted the condensation and diazotization cyclization reactions. Furthermore, increasing the reaction temperature (from 400 to 800 °C) significantly increased the yields of heterocycles-N, while the yields of amines and amides decreased sharply due to dehydration reaction. As analyzed above, the possible nitrogen migration mechanism and involved chemical reactions were elucidated. These findings provides insights for generating high value-added N-containing chemicals and N-doped carbon materials during N-rich pyrolysis.
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JOURNAL OF MOLECULAR LIQUIDS
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2024
·
IF 5.3
Ke Bei,Youyan Wang,Dan Yang,Qizhi Shao,Xiangyong Zheng,Min Zhao,I-Ming Chou,Jun Kikuchi,Zhiyan Pan
This study used a high pressure optical cell (HPOC) combined with a heating/cooling stage, a pressure device, and a laser Raman spectrometer to investigate the volume expansion (VE) of CO 2 + tetradecane and CO 2 + hexadecane mixtures under geological storage conditions. Abrupt changes in VE were observed near the CO 2 critical point (CP), which is assumed to be ubiquitous in CO 2 + long-chain alkane mixtures with ≥14 carbon alkanes. This is due to the critical anomaly of the thermodynamic behavior of the mixture near the CP of CO 2 , which inhibits the VE of CO 2 + long-chain alkanes at lower temperatures. In addition, four machine learning (ML) algorithms, including backpropagation neural network (BPNN), K-nearest neighbors (KNN), random forest (RF), and support vector regression (SVR), were applied to predict the volume expansion factor (VEF). The BPNN model provided much higher robustness and accuracy with correlation coefficient ( R 2 ) >0.98 and mean square error ( MSE ) <0.03, which indicates a strong agreement between the predicted result and matching experimental data. We concluded that a predictive framework built using ML could provide rapid predictions of the volume change curve or curved surface of CO 2 + organic mixtures under various temperature and pressure conditions.
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JOURNAL OF CHEMICAL THERMODYNAMICS
·
2022
·
IF 3.269
Pan Zhang,Yanxi Ji,Wenya Li,Lihua Xu,Lemeng Wang,Dong Fu
The viscosities of N -(2-aminoethyl)ethanolamine (AEEA), 1,4-butanediamine (BDA) and N-methyl- 1,3-propane- diamine (MAPA) activated 2- diethylaminoethanol (DEAE) aqueous solutions were measured at temperatures ( T ) from 303.2 K to 323.2 K, respectively. The DEAE mass fractions ( w DEAE ) and the other three amines ( w AEEA / w BDA / w MAPA ) are 0.300 to 0.500 and 0.050 to 0.150 respectively. The Weiland equation was used to calculate the viscosity of these three solutions, and the calculation results were satisfied with data of the experimental results. With the aid of experimentally determined viscosity data, the activation energy ( E a) of these three solutions was predicted through the Arrhenius formula. With the help of the viscosity data and the diffusion coefficient model of CO 2 in water, the CO 2 diffusion coefficient ( D CO2 ) in these three solutions was calculated. The quantitative relationship between the calculated values (viscosity, activation energy and diffusion coefficient) and the operation conditions (solution mass fraction and temperature) was analyzed. Our results show that the DEAE-BDA absorbent has better application potential due to its lower viscosity, higher CO 2 diffusion coefficient and lower activation energy.
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TETRAHEDRON
·
2014
·
IF 2.817
Dazhuang Miao,Xuesong Shi,Guozhen He,Yao Tong,Zengqiang Jiang,Shiqing Han
N -(2-Chloro-phenyl)-2-halo-benzamides (halo=I/Br/Cl) as substrates were used for the one-pot synthesis of 2-arylbenzoxazole derivatives via copper-catalyzed intermolecular C–N/intramolecular C–O couplings with primary amines . This aryl amination offers clean reaction conditions and easy work-up in good yields by using CuI as catalyst, readily available 8-hydroxyquinoline as ligand, K 3 PO 4 as base, DMF as solvent.
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ACS Omega
·
2026
·
IF 5.2
Jing Zeng,Yuting Zhao,Yaxin Chen,Kun Wu,Changlei Yang,Ying Wu,Guanglong Pang,Miao Zhang,Huaixiu Wen,Zhen Wang,Xue Peng
Alzheimer’s disease (AD) is a neurodegenerative disease (NDD) characterized by complex pathogenesis and remains incurable to date. Emerging evidence has demonstrated that mitochondrial dysfunction not only serves as a central component in AD initiation but also precedes other pathological processes, thereby playing a pivotal role in both the pathogenesis and progression of AD. Previous studies have confirmed that N-salicyloyl tryptamine derivatives can regulate mitochondrial function and effectively treat NDDs. Among them, compound N2 showed the best efficacy. This study first applied compound N2 to the treatment of AD and confirmed that it exerts anti-AD effects by upregulating nuclear factor erythroid 2-related factor 2 (Nrf2) and enhancing the activity of mitochondrial complex I (MCI). The results showed that N2 improved mitochondrial dysfunction and neuro-inflammation in PC12 or BV2 cells. N2 was also shown to alleviate anxiety, cognitive impairment, neuronal damage, and amyloid-β (Aβ) pathological deposition in scopolamine-induced male Kunming mice. Mechanistic studies indicate that N2 can reverse mitochondrial damage induced by rotenone (MCI inhibitor), as evidenced by reduced ROS levels and increased ATP levels; it also upregulates Nrf2 protein expression. These findings collectively indicate that N2 is a highly valuable anti-AD mitochondrial function regulator, providing a new strategy for the efficient treatment of AD.
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