Chem Catalysis
·
2022
·
IF 0
Xianhao Zhang,Huijuan Jing,Shiming Chen,Bing Liu,Liang Yu,Jianping Xiao,Dehui Deng
Summary Cyclohexanone oxime (CHO), a key C=N organic compound in the manufacture of nylon 6, is conventionally synthesized via a multistep process that consumes expensive NH 3 and H 2 under harsh conditions. Herein, we report the direct electro-synthesis of CHO from low-cost NO, H 2 O, and cyclohexanone over a carbon catalyst under ambient conditions. A high Faradaic efficiency of 44.8% and a formation rate of 10.7 mg cm −2 h −1 for CHO were achieved at −0.4 V versus the reversible hydrogen electrode through optimizing the surface hydrophobicity of the catalyst to facilitate diffusion of reactants. Controlled experiments and 15 N-labeling tests verified that the nitrogen in the CHO product originates from NO. Density functional theory calculations showed that the armchair edge of carbon could be the active site with a reaction mechanism following NO → NO∗ → HNO∗ → HNOH∗ → NH 2 OH → CHO. This work suggests a direct, green, and low-cost synthesis strategy for high-value CHO from pollutant NO.
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JOURNAL OF MEMBRANE SCIENCE
·
2015
·
IF 5.056
Liang Cheng,Li-Ping Zhu,Pei-Bin Zhang,Jian Sun,Bao-Ku Zhu,You-Yi Xu
Here we demonstrate the tunable molecular selectivities and corresponding mechanisms of poly(N-vinyl imidazole) (PVI) gel-filled membranes prepared by UV initiated graft polymerization of N-vinyl imidazole from ultraporous polysulfone (PSf) substrate. The separation performance was investigated in detail by extensive filtration tests with various organic molecules in water of varying pH and also in salt or ethanol aqueous solution. The variation of membrane water permeability and solute rejection with the feed pH was attributed to the sensitive pore size and charge characteristics of the membranes upon reversible protonation of the confined PVI gel. The separation results discerned three main mechanisms, i.e. size exclusion (sieving), electrostatic repulsion (Donnan exclusion) and adsorption. The rejection of the neutral molecules and the large dye molecules was mostly ascribed to size exclusion, while that of the small charged solutes was dominated by the electrostatic interactions including repulsion for cationic ones and attraction for anionic ones (causing specific adsorption). Typically, at pH 3 the protonated membranes rejected ~90% of the small cationic Vitamin B 1 (VB 1 ) and 100% of the anionic Sunset Yellow (SY) before adsorption saturation, in contrast to less than ~20% rejection of the neutral Vitamin B 2 (VB 2 ) having similar molecule size. In the high concentration salt or ethanol solution the membranes still maintained molecular sieving capability. Most notably, the separations of solute mixtures were indeed achieved, depending on the membrane parameters, the solute characteristics as well as the filtration conditions. The PVI gel-filled membranes developed in this work are promising in some specified or environment-sensitive molecular level separations.
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Materials Today Communications
·
2024
·
IF 3.7
Yanhua Li,Shuhuan Wang,Kuo Zhang,Dongjia Wang,Qun Li,Yuekai Xue
Herein, the N-doped Ti 3 C 2 /TiO 2 nanostructure has been synthesized via hydrothermal treatment and following annealing in NH 3 . TiO 2 nanoparticles in-situ grow on the surface of Ti 3 C 2 spontaneously, resulting in the stable electron transport between TiO 2 and Ti 3 C 2 . Besides, Ti 3 C 2 nanosheets as conductive substrates make up for the poor conductivity of TiO 2 . The doping of N in Ti 3 C 2 /TiO 2 composite further improves the electrical conduction. The ultimate N-doped Ti 3 C 2 /TiO 2 composite achieves a higher specific capacitance of 737.4 F g −1 than Ti 3 C 2 (324.4 F g −1 ) at 0.5 A g −1 . More importantly, the composite displays a high specific capacitance retention of 81 % over 12,000 cycles. Besides, the assembled symmetrical supercapacitor (SSC) manifests an excellent specific capacitance of 236.4 F g −1 at 1 A g −1 and a comparable energy density of 32.8 Wh kg −1 at the power density of 500 W kg −1 . This work provides promising guidance for the fabrication of durable electrodes for energy storage application.
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REACTIVE & FUNCTIONAL POLYMERS
·
2025
·
IF 5.1
Chang-Yuan Cheng,Yong Xiang,Jing-Ping Sun,Wen-Cai Bai,Zhou-Xuan Zang,Ou-Yang Liu,Li Xu
In this study, we crafted nitrogen-laden microspheres known as PEI-GA, employing a straightforward, single-step synthesis at ambient temperature. We further validated their capacity as autonomous adsorbents, capable of achieving efficient, targeted, and swift extraction of gold ions (Au(III)) from aqueous media. The high nitrogen content of PEI, combined with its electrochemical adsorption ability, enables effective adsorption and reduction of Au(III) ions into gold nanoparticles, significantly enhancing the adsorption capacity and selectivity. PEI-GA exhibits an ultra-fast adsorption rate, achieving over 99 % Au(III) recovery in just 1 min at a concentration of 100 mg/L (m/V = 0.5 g/L). Moreover, even at higher concentrations (300 mg/L), the process only takes 5 min. The maximum adsorption capacity of PEI-GA reaches 2078 mg/g, following the Langmuir model and pseudo-second-order kinetics. PEI-GA also demonstrates excellent selectivity and recyclability, recovering over 95 % of gold ions from simulated e-waste solutions and maintaining 90 % recovery efficiency after five cycles. DFT calculations suggest that AuCl₄ − tends to form multicentric coordination with N atoms in PEI-GA. This study highlights the cost-effectiveness of PEI-GA for Au(III) recovery, which can be further optimized through calcination or regeneration.
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产品关联
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高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
·
2021
·
IF 3.498
Jie Chen,Deyu Bao,Qiang Sun,Wei-Di Liu,Can Liu,Jun Tang,Lei Yang,Dali Zhou,Matthew S. Dargusch,Zhi-Gang Chen
To achieve the optimized performance and the widespread application of thermoelectric materials , it is crucial to decouple the highly interrelated thermoelectric parameters of materials. In this study, we illustrate that phonon and carrier transport properties of n-type Bi 2 Te 3 -based composites can be simultaneously optimized through alloying Cu 2 Se. Owing to the chemical reactions between the Bi 2 Te 3 matrix and the Cu 2 Se additives during the sample preparation, the carrier concentration and density-of-states effective mass can be tuned to optimize the carrier transport properties, while the lattice thermal conductivity can be reduced by introducing hierarchical structures including point defects , Cu 7 Te 5 inclusions, phase boundaries and localized Te-deficient regions. As a result, an enhanced thermoelectric performance is achieved compared with pristine Bi 2 Te 3 . Our study indicates the alloying Cu 2 Se can synergistically control the thermoelectric properties of Bi 2 Te 3 .
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CHINESE JOURNAL OF POLYMER SCIENCE
·
2015
·Vol. 33
·期 11
·1618-1624
·
IF 1.835
Hu Wei,Cao Jing,Huang Yi-ling,Liang Sai
The anionic polymerization of N -vinylcarbazole (NVC) by using optically active anionic initiators such as the lithium salts of ( S )-1-(9H-fluoren-2-yl)-4-isopropyl-4,5-dihydrooxazole (( S )-1-FIDH) and ( S )-2-(9H-fluoren-2-yl)-4- isopropyl-4,5-dihydrooxazole (( S )-2-FIDH) and complexes of (-)-Sparteine with n -butylithium (n-BuLi-(-)-Sp) or fluorenyl lithium (FILi-(-)-Sp) was achieved. The yield and specific rotation of poly( N -vinylcarbazole)s (poly(NVC)s) were considerably affected by the molar ratio of ( S )-FIDH to NVC. The highest yield and specific rotation were obtained with Li- ( S )-1-FIDH as an initiator, with a molar ratio of monomer and initiator [M]/[I] = 10/1. The effects of the chiral initiators, type of solvent and the polymerization temperature were investigated. The obtained optical activity of polymers was attributed to asymmetric induction of the chiral initiators.
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JOURNAL OF MOLECULAR LIQUIDS
·
2021
·
IF 6.165
Qian Zhang,Yongzhong Jia,Jinhe Sun,Pengrui Zhang,Chaochi Huang,Mingyong Wang,Zixuan Xue,Ciming Wang,Fei Shao,Fengtai Tong,Yilin Xiao,Yan Jing
Azacrown ethers contain multiple coordination sites, which show specific complexation to alkali metal ions . In this research, a neoteric liquid-liquid extraction system was investigated for the selective separation of lithium isotope using N -phenylaza-15-crown-5 (Ph-N15C5) as chelating agent and [BMIm][NTf 2 ] and anisole as extraction solvent. The effects of the counter anions of lithium salt , concentrations of crown ether , temperature, extraction equilibrium time and concentrations of lithium salt solution on the separation of lithium isotope with Ph-N15C5 were studied. The maximum extraction efficiency of lithium ions was 41.54% and the maximum single-stage separation factor (α) of 6 Li/ 7 Li obtained in the present study was 1.025, indicating that the lighter isotope 6 Li was enriched in organic phase while the heavier isotope 7 Li was concentrated in the aqueous phase. The complexation ratio of the lithium crown ether complex was determined as 1:1 by the slope analysis method. The lithium ions in the aqueous phase were extracted into the organic phase to form [Li(Ph-N15C5)] + complex. The thermodynamic data obtained at different temperatures demonstrated that lithium isotope exchange was a spontaneous exothermic process , and lowering the temperature was beneficial to increase the separation factor. In addition, the system reached the extraction equilibrium after 60 min. This high efficiency and green liquid-liquid extraction system has potential application in lithium isotope separation.
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JOURNAL OF ORGANIC CHEMISTRY
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2021
·
IF 4.354
Haopeng Wu,Chukai Shao,Di Wu,Liang Jiang,Hongquan Yin,Fu-Xue Chen
A highly regioselective protocol for intermolecular thiocyanation-amination of alkynes by N-thiocyano-dibenzenesulfonimide (NTSI) as the SCN and nitrogen sources has been developed. A C–S bond and C–N bond are simultaneously constructed in only one step. The reaction under simple mild conditions features a broad substrate scope, atom economy, high yields (up to 94%), and excellent functional group tolerance.
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PubMed
高影响因子
BIORESOURCE TECHNOLOGY
·
2014
·
IF 5.039
Cuiping Chen,Wenjun Zhou,Daohui Lin
N-nitrosodimethylamine (NDMA) is an emerging carcinogenic disinfection by-product in water environment. Biochars utilized as sorbents for the removal of NDMA from aqueous solution, and the sorption characteristics and mechanism were investigate. Biochars were prepared from bamboo, rice straw and wood sawdust at 300–700 °C. The pseudo-second-order model provided the best fit for the sorption kinetics of NDMA onto biochar and the sorption isotherms were described best with the Slips model. Biochar produced at 500 °C removed NDMA from aqueous solution relatively efficiently, and the bamboo char demonstrated the best sorption potential among the three types of biochars. Solution chemistry such as pH and metal ions did not show obvious effect on NDMA removal. Three sorption mechanisms are suggested for NDMA sorption onto biochars, H-bond attraction between N O and the O-containing moieties, hydrophobic force between CH 3 and the ordered graphitic structure, and partition process of NDMA into the non-carbonization part of biochar.
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PubMed
高影响因子
EUROPEAN POLYMER JOURNAL
·
2018
·
IF 3.741
Xi Chen,Xiaojun Liu,Congcong Miao,Pengfei Song,Yubing Xiong
Inimer bears a polymerizable vinyl group and a reactable group, and thus has great potentials in the synthesis of branched and functional polymers. Herein, a strategy was developed for the synthesis of ionic liquid (IL)-like inimer containing a trithiocarbonate moiety and a styryl group. The newly-developed IL-like inimer could be facilely achieved via the neutralization reaction using a carboxyl-contained chain transfer agent (CTA) and an alkaline IL monomer. The IL-like inimer was characterized through proton and carbon nuclear magnetic resonance spectroscopy ( 1 H and 13 C NMR), Flourier transform infrared spectroscopy (FT-IR) and Mass spectroscopy. Moreover, the reversible addition-fragmentation chain transfer (RAFT) polymerization of N-isopropylacrylamide (NIPAM) mediated by the as-prepared IL-like inimer was investigated. The results revealed that branched PNIPAM with tunable molecular weight and degree of branching (DB) could be prepared. Additionally, lower critical solution temperature (LCST) of branched PNIPAM could be adjusted through the feed ratio of IL-like inimer and the monomer in the polymerization process. As a result, our study offers a new technique for the design of functional inimer, as well as broadens the application of ILs in the polymer field.
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Heliyon
·
2023
·Vol. 9
·期 4
·e15357
·
IF 4
Xiufeng Wu,Zhaoliu Cao,Jiang Ni,Xiaoyuan Zheng,Lizhen Zhu,Xin wang,Juan Lv,Shijun Zhou,Yongjuan Ding,Ruirong Wu
Mixing different kind inhalation medications for simultaneous inhalation is widely used in the treatment of chronic respiratory diseases, and it can minimize the administration time and improve patient adherence. To our knowledge, it is unclear whether beclomethasone (BDP, Clenil®) can bemixed with acetylcysteine (NAC, Fluimucil®), because the in vitro physico-chemical compatibility and aerosol characteristics of the mixture are unknown. In this study, we investigated physical compatibility, including the appearance, pH, osmotic pressure and chemical stability, as well as aerosol characteristics, including particle size corresponding to 10%/50%/90% of the cumulative percentage of total particle volume ( X 10/ X 50/ X 90), volume median droplet diameter (VMD), mass median aerodynamic diameter (MMAD), fine particle fraction (FPF), fine particle dose (FPD) and geometric standard deviation (GSD), delivery rate, and total delivery of the above solutions. After mixing, there were no significant changes in visual appearance, pH, osmolality and drug content of the mixtures at room temperature for 12 h. The FDP of BDP in the mixture decreased by 16.49%, whereas the NAC increased by 10.85%. The delivery rates of BDP and NAC in the mixture decreased by 66.05% and 45.54%, and total delivery increased by 13.20% and 25.29%, respectively. However, the MMAD, FPF, particle size and GSD of the mixture were almost unchanged. We demonstrated that these admixtures are physico-chemically compatible but that coadministration of beclomethasone with acetylcysteine can markedly affect output and aerosol characteristics.
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PubMed
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2022
·
IF 5.723
Yan Li,Mengna Ding,Guoxiang Yang,Lei Wang,Liulin Luo,Yingchun Miao,Yuning Huo
Acinetobacter baumannii ( A. baumannii ) was widely existed in medical wastewater and easily induced infections to threaten the human healthy. We herein reported Ag/CoO-N photocatalyst composites for effective inactivation of A. baumannii . Ag/CoO-N composites were prepared by N-doping to CoO crystal in supercritical fluid followed with photo-reduction of Ag under visible-light irradiation. N-species was incorporated in the crystal structure of CoO, on which uniform Ag nanoparticles were stably deposited. Thus, the satisfactory photocatalytic sterilization of A. baumannii irradiated by visible-light irradiation was attributed to the high capability of light trapping and the efficient separation of photo-charges. Due to photo-induced electrons as the main active species, Ag nanoparticles and CoO-N synergistically realized mineralization of cell membrane, which lead K + ions leak from cell to crack structure of bacteria, the decrease of genetic materials, and the cripple of the self-repair function in bacteria, resulting in the final cell death.
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