JOURNAL OF HAZARDOUS MATERIALS
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2021
·
IF 10.588
Xingyu Fang,Lu Gan,Linjie Wang,Han Gong,Lijie Xu,Ying Wu,Haiqin Lu,Shuguang Han,Juqing Cui,Changlei Xia
In this study, mixed metal cobalt zinc oxide embedded nitrogen enriched porous carbon composites (CoZnO-PC) were prepared via pyrolyzing polyvinylpyrrolidone (PVP) encapsulated Co, Zn-bimetal centered zeolitic imidazolate frameworks (ZIF). The prepared composites were then used to activate peroxymonosulfate (PMS) for bisphenol A (BPA) removal in water. When mole ratio of Co/Zn was 2/1, the resulted Co 2 Zn 1 O-PC possessed spinel structure with prominent degradation capability, in which the introduction of Zn accelerated the PMS activation performance of Co through establishing bimetal synergistic interactions. Both radical and non-radical activation pathways were existed in the Co 2 Zn 1 O-PC/PMS system, in which Co 2 Zn 1 O dominated the radical pathway whereas PC dominated the non-radical way. Since PVP contained abundant nitrogen atoms and could form strong coordination interactions with the ZIF precursor, the introduction of PVP in the ZIF precursor prevented pore collapsing during pyrolysis process , as well as enhancing the nitrogen content in the pyrolzed composites, which significantly promoted the generation of singlet oxygen. With combined pathways, the Co 2 Zn 1 O-PC/PMS system showed a wide pH application range with promising mineralization rate. Meanwhile, the spinel-structured Co 2 Zn 1 O-PC was magnetically separable with desirable recyclability . This study presents a novel composite with remarkable performance for the removal of refractory organic pollutants in municipal wastewater .
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JOURNAL OF SOLUTION CHEMISTRY
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2020
·Vol. 49
·期 4
·423-457
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IF 1.273
Cai Guangming,Yang Shaoqi,Wang Xinxin,Zhou Qing,Xu Junli,Lu Xingmei
2-hydroxy- N -(2-hydroxyethyl)- N -methylethanaminium methanesulfonate ([BHEM][mesy]) displayed good ability for separating cellulose from biomass material in previous works. In order to have a better understanding of the structure–property relationship and facilitate further potential applications in industry, it is necessary to obtain more data for the physicochemical properties of [BHEM][mesy] and its mixtures. In this work, the densities ( ρ ) and viscosities ( η ) of [BHEM][mesy] + solvents (water, methanol, ethanol, n -propanol and isopropanol) mixtures were measured at six temperatures from (298.15 to 323.15) K over the full molar composition range and fitted by an empirical quadratic equation and Vogel–Fucher–Tammann (VFT) equation. Moreover, the excess molar volumes ( V E ) and viscosity deviation (Δ η ) of five binary mixtures were calculated and correlated by the Redlich–Kister equation. In addition, the apparent molar volumes ( \({V}_{\varphi }\) ) and partial molar volumes ( \(\stackrel{-}{V}\) ) of [BHEM][mesy] and solvents were also calculated and all these physicochemical property data (density, viscosity, excess molar properties as well as the apparent molar properties) are discussed in terms of the structure and interaction of binary mixtures.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2020
·
IF 3.573
Jincheng Mu,Jianfang Liu,Zhenzhen Ran,Muhammad Arif,Min Gao,Chen Wang,Shengfu Ji
MOF-808(Zr) with the coordinated unsaturated (CUS) Zr4+ centers was synthesized by the thermal reflux method, and a series of Au/MOF-808(Zr) catalysts with different Au loading percentages have been prepared by the impregnation–reduction method. The related X-ray diffraction, Fourier transform infrared spectroscopy, high-resolution transmission electron microscopy, X-ray photoelectron spectroscopy, N2 adsorption–desorption, Inductively coupled plasma-mass spectrometry, and NH3 temperature-programmed desorption characterizations have been undertaken to understand the structure of catalysts. The catalytic activity in CO2 with aniline/H2 to N-methylation and N-formylation has been studied in a batch reactor. Results show that the MOF-808(Zr) structures in catalysts are of high quality and damage-free. The Au nanoparticles (NPs) are highly dispersed on the surface of the MOF-808(Zr) cage with a mean size of 2–20 nm. Also, the catalysts could catalyze the conversion of CO2 with aniline/H2 to N-methylation and N-formylation products with a high efficiency. With a 3.0 wt % Au/MOF-808(Zr) catalyst, the conversion of aniline is 18.4%, and the selectivity of N-methylaniline is 80.9% and that of N,N-dimethylaniline is 19.1%. The preliminary reaction mechanism and the critical role of CUS were also studied. It is determined that H2 is adsorbed and activated on Au NPs. CO2 is adsorbed on the CUS Zr4+ acidic sites and O2– basic sites. The primary and secondary amines are adsorbed on the CUS Zr4+ acidic sites, where they react with CO2 and H2 to form N-formamide. Subsequently, N-formamide reacts with activated H2 to yield N-methylamine.
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INTERNATIONAL JOURNAL OF ENERGY RESEARCH
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2020
·Vol. 44
·期 6
·4875-4887
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IF 3.741
Zhixiu Yang,Xiaofei Guo,Guojie Zhang,Ying Xu
Summary Porous carbon materials have been widely used for CO 2 adsorption, but their preparation was subject to conditions such as raw material cost, activator corrosion, and temperature. In this study, nitrogen-doped porous carbonaceous adsorbents were prepared in a low temperature region (400-550°C) by one-step composite nitrogen doping method, using low-cost oil residue as raw materials and less corrosive NaNH 2 as activator. The CO 2 adsorption performances of the prepared N-doped porous adsorbents were systematically explored. The results showed that optimal oil residue-derived carbonaceous adsorbent owned excellent amount of CO 2 adsorption up to 3.51 and 5.63 mmol/g at 298 and 273 K under 1 bar, respectively. It was discovered that the congenerous influences of porous structure, nitrogen content and V n of the adsorbent affected their CO 2 adsorption performances under 1 bar. Importantly, these oil residue porous carbonaceous adsorbent also was verified owning fine selectivity of the CO 2 over N 2 (15.7), which attributed to its high V n and nitrogen content. Furthermore, optimal sample OAC-500-2.5 owned medium Q st (21-26 kJ/mol), which was beneficial practical application. This work may inspire new sparks on novel nitrogen-doped adsorbent with inexpensive precursor, low activation temperature and simple preparative tactic, indicating that the nitrogen-doped sample is promising in the practical situation of CO 2 adsorption.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2020
·
IF 2.369
Yajun Li,Xiaofang Li,Kui Wu
In this work, the solubility of N,N-dibenzylhydroxylamine (DBHA) in 17 pure solvents, including methanol, ethanol, n-propanol, n-butanol, acetone, ethyl acetate, dichloromethane, acetonitrile, isopropanol, n-octanol, cyclohexanone, 1,2-dichlorobenzene, toluene, isobutanol, n-pentanol, 1,2,4-trichlorobenzene, and tetrahydrofuran, was determined by a static gravimetric method with the temperature ranging from 273.15 to 323.35 K under atmospheric pressure. The solubility of DBHA was positively related to temperature in all selected solvents. Besides, the experimental solubility data were correlated with four thermodynamic models, i.e., the modified Apelblat equation, λh equation, nonrandom two-liquid (NRTL) equation, and the Wilson equation. The results indicated that all of the models could give satisfactory results and the NRTL equation provided the best fitting result. Furthermore, the dissolution thermodynamic parameters in the used solvents, including the Gibbs energy (ΔdisG), molar enthalpy (ΔdisH), and molar entropy (ΔdisS), were calculated according to the Wilson model, and it turned out that the dissolution process of DBHA was endothermic.
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FUEL PROCESSING TECHNOLOGY
·
2022
·
IF 8.129
Qin Wen,Dongxu Tian,Zequan Zeng,Fei Qi,Zhanggen Huang
Fe-N-C catalysts with magnetism were successfully synthesized through one-step heat treatment of ferrosoferric oxide and covalent organic frameworks composite (Fe 3 O 4 @COF) as heterogeneous catalysts for persulfate (PS) activation and 2,4-dichlorophenol (2,4-DCP) degradation. The morphologies, compositions and active sites were adjusted by changing the pyrolysis temperature. The catalyst prepared at 900 °C showed excellent activity with 2,4-DCP removal of 90% in 60 min, recycling convenience and regeneration stability. Large surface area (342 m 2 g −1 ) and hierarchical porous structure benefited PS activation. It was proved that the radical and non-radical mechanisms coexisted in Fe-N-C-900/PS system with the results of quenching and electrochemical experiments. Roles of graphitic N and Fe-N X were distinguished. Graphitic N and Fe-N X sites palyed an prominent part in the non-radical activation process , in which Fe-N X was closely related to the electron transfer activation mechanism. Density functional theory (DFT) calculation further verified that the Fe N 2 was the key site for PS activation. 2,4-DCP degradation was proved to be a toxicity-attenuation process according to the biotoxicity analysis. The effects of several operating parameters and degradation of different model pollutants were also systematically evaluated, and possible activation mechanism was proposed.
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BIOORGANIC & MEDICINAL CHEMISTRY
·
2017
·
IF 2.93
Xiaoyan Han,Yifan Zhong,Guan Zhou,Hui Qi,Shengbin Li,Qiang Ding,Zhenming Liu,Yali Song,Xiaoqiang Qiao
A new series of thirteen N -(carbobenzyloxy)- l -phenylalanine and N -(carbobenzyloxy)- l -aspartic acid- β -benzyl ester compounds were synthesized and evaluated for antiproliferative activity against four different human cancer cell lines: cervical cancer (HeLa), lung cancer (A549), gastric cancer (MGC-803) and breast cancer (MCF-7) as well as topoisomerase I and IIα inhibitory activity. Compounds ( 5a , 5b , 5e , 8a , 8b ) showed significant antiproliferative activity with low IC 50 values against the four cancer cell lines. Equally, compounds 5a , 5b , 5e , 5f , 8a , 8d , 8e and 8f showed topoisomerase IIα inhibitory activity at 100 μM with 5b , 5e , 8f exhibiting potential topoisomerase IIα inhibitory activity compared to positive control at 100 μM and 20 μM, respectively. Conversely compounds 5e , 5f , 5g and 8a showed weaker topoisomerase I inhibitory activity compared to positive control at 100 μM. Compound 5b exhibited the most potent topoisomerase IIα inhibitory activity at low concentration and better antiproliferative activity against the four human cancer cell lines. The molecular interactions between compounds 5a – 5g , 8a – 8f and the topoisomerase IIα (PDB ID: 1ZXM ) were further investigated through molecular docking. The results indicated that these compounds could serve as promising leads for further optimization as novel antitumor agents.
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Materials Horizons
·
2023
·Vol. 10
·期 12
·5712-5719
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IF 13.3
Mengmeng Wang,Yunmei Du,Shuangshuang Li,Xiaoli Sun,Bin Li,Yuanxiang Gu,Lei Wang
The N-doping strategy plays a vital role in optimizing electrocatalytic performance, but it often requires high-temperatures accompanied by the emission of irritating gases, which is contrary to the concept of energy saving and environmental protection. Based on this, this work innovatively uses the quenching of waste heat and the non-equilibrium state of materials to realize controllable N-doping. Notably, N dopants stimulate metal-like electroconductivity and accelerate the alkaline HER kinetics by optimizing the electronic structure of Ru2P. Surprisingly, the hydrophilic Ru core and the N-Ru2P shell with a low HER reaction energy barrier synergistically expedite hydrogen release. As anticipated, the current density of N-Ru2P@Ru (963 mA cm−2) is 2.6-fold that of Pt/C (359 mA cm−2) at 150 mV. Overall, the novel N-doping technology greatly simplifies material preparation procedures and reduces energy consumption. Moreover, this unique N-doping strategy provides a new idea for optimizing the catalyst structure and reaction kinetics.
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International Journal of Greenhouse Gas Control
·
2019
·
IF 3.231
Fan Cao,Hongxia Gao,Qian Xiong,Zhiwu Liang
CO 2 absorption performance for various blended N ,N- dimethylethanolamine (DMEA) solutions in the presence of absorption promoters including Monoethanolamine (MEA), Piperazine (PZ), 2-(Ethylamino)ethanol (EAE), 2-(Methylamino)ethanol (MAE) and 2-Amino-2-methyl-1-propanol (AMP) was investigated in terms of CO 2 absorption flux by using a polytetrafluoroethylene (PTFE) hollow fiber membrane contactor. The experimental results show that the CO 2 absorption flux increases with a reasonable increase in liquid velocity, liquid temperature and total amine concentration. Also, the CO 2 absorption flux can increase by increasing gas velocity, CO 2 partial pressure but decrease with the increased lean CO 2 loading. In addition, it can be found that all of the investigated activated amines can improve the CO 2 absorption flux of aqueous DMEA solution. For fresh amine solution, the order of CO 2 absorption flux for the investigated amine blends can be ranked as: DMEA < DMEA + AMP < DMEA + MEA < DMEA + EAE < DMEA + MAE < DMEA + PZ. By contrast, for the amine solution with CO 2 loading of over 0.3 mol/mol, the order has also changed accordingly and can be ranked as: DMEA < DMEA + AMP < DMEA + EAE < DMEA + MAE < DMEA + MEA < DMEA + PZ. The DMEA + PZ mixture presents a significant improvement up to 52.44% in CO 2 absorption flux compared to that of single DMEA solution, and can be considered as a promising alternative for CO 2 capture.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2018
·
IF 3.141
Fan Cao,Hongxia Gao,Haipeng Li,Zhiwu Liang
N,N-Dimethylethanolamine (DMEA) is a promising absorbent due to the relative higher reaction rate and high capacity for CO2 capture. In this work, the CO2 absorption performance into aqueous DMEA solution using a polytetrafluoroethylene (PTFE) hollow-fiber membrane contactor (HFMC) was investigated experimentally and numerically. The CO2 absorption fluxes were determined under various important operating parameters, including liquid velocity, gas velocity, liquid feed temperature, CO2 partial pressure, and CO2 loading in liquid phase. In addition, a 2D steady-state mathematical model was established to predict the CO2 absorption flux in two operation modes, nonwetted and partially wetted modes, and was validated by using the CO2 absorption into water and aqueous MEA solution. The experimental and simulated results revealed that the CO2 absorption flux can be enhanced by increasing liquid velocity, liquid-phase temperature, and amine concentration in a moderate range. Also, the CO2 absorption flux will increase with the increasing gas velocity and CO2 partial pressure but decrease with increasing CO2 loading in the liquid phase. In addition, the membrane wetting can cause a severe deterioration in the CO2 absorption performance even with a slight membrane wetting. The CO2 absorption fluxes for CO2 absorption into DMEA solutions show the good agreement with or are closer to the simulated data with the membrane wetting of 10% under the same operational conditions, with the average absolute relative deviation (AARD) of 5.02%. Furthermore, the obtained radical and axial CO2 concentration profiles from the mathematical model were also discussed to further understand the CO2 absorption process.
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MACROMOLECULAR CHEMISTRY AND PHYSICS
·
2019
·Vol. 220
·期 9
·1900022
·
IF 2.622
Wenxiu Zhang,Xianhong Zhang,Yuhong Ma,Dong Chen,Wantai Yang
With UV–vis absorption in the range of 270–435 nm, 4-( N , N -diphenylamino)benzaldehyde (DPAB) takes efficient photoreduction quench with 4-cynao-4-(phenylcarbonothioylthio)pentanoic acid (CTP). The polymerization rates of methyl methacrylate (MMA) are 0.019, 0.056, and 0.102 h −1 at 33, 40, and 50 °C, respectively, in the presence of DPAB and CTP under visible-light irradiation. Dark reaction produces no PMMA at 50 °C for 120 h. The living feature is demonstrated by linearly increasing M n with the monomer conversions and narrow polydispersity index (PDI), chain extension, and block polymerizations with benzyl methacrylate (BnMA) and poly(ethylene glycol) monomethyl ether methacrylate (PEGMA). With PMMA-CTP ( M n = 6800, PDI = 1.17), chain extension gives PMMA with M n = 15 900 and PDI = 1.15. With PMMA-CTP ( M n = 6000, PDI = 1.21) as macro-RAFT, PMMA- b -PBnMA of M n = 12 600 (PDI = 1.44) and M n = 18 500 (PDI = 1.31) are prepared. These results support that there is a positive synergistic effect between polymerization temperature and visible-light irradiation on the photo-RAFT without losing the living features.
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CHEMOSPHERE
·
2018
·
IF 4.427
Xiaohua Ren,Jinkui Feng,Pengchao Si,Lin Zhang,Jun Lou,Lijie Ci
3D porous sulfur and nitrogen co-doped graphene aerogel has been fabricated by a facile one-pot process. Both experimental and theoretical studies have demonstrated that sulfur and nitrogen co-doping could synergistically enhance the catalytic performance for activating peroxydisulfate (PDS) compared to the original and N doped graphene aerogels. The ratio of sulfur/nitrogen in the aerogel can be controlled by regulating the additions of thiourea and urea sources, and the aerogel with the S/N ratio of about 1:2.5 shows a better catalytic effect due to more significant changes in the electrostatic potential and the surface charge distribution, as revealed by the theoretical simulations. The radical quenching tests indicated that both SO 4 · - and ·OH radicals could be formed in the SN-rGO aerogel + PDS system and contribute most to RhB degradation.
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