RUSSIAN JOURNAL OF ORGANIC CHEMISTRY
·
2022
·Vol. 58
·期 6
·837-843
·
IF 0.862
Gu Zhengyu,Xue Feng,Yu Jiale,Ju Shengui
Abstract N -Aryl anthranilic acid drugs have been synthesized by a simple, environmentally friendly, low-cost, and high-yielding modified Ullmann coupling reaction protocol using potassium 2-bromobenzoate, substituted anilines, and copper acetate in tetrabutylphosphonium chloride ([TBP]Cl) ionic liquid. The optimal conditions have been found and applied to the synthesis of N -aryl anthranilic acid drugs at 170°C. Mass spectrometry, X-ray crystallography, and proton nuclear magnetic resonance were used to describe the structure of the products. Copper(I) complex catalyst was used as a starting catalyst for the Ullmann reaction because of the good fluidity and homogeneity in [TBP]Cl ionic liquid. Meclofenamic, mefenamic, clofenamic, and flufenamic acids were synthesized efficiently using the proposed general procedure. The distinct advantages of the described protocol are operational simplicity, cleaner reaction, high selectivity, excellent yield, rapid conversion, easy preparation, and the use of a low-cost catalyst.
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Molecular Catalysis
·
2022
·
IF 5.089
Xiao-Chao Chen,Lin Guo,Guang-Hui Shi,Kai-Chun Zhao,Yong Lu,Ye Liu
Carbon dioxide (CO 2 ) was found to serve as a novel and green catalyst for the first time in N -formylation of amines with N, N -dimethylformamide (DMF), wherein only the aliphatic amines were applicable to afford the formamides in the yield of 71∼95%. The isotope labeling experiment with DMF- d 7 indicated that the N -formyl group in the formylated product was originated from DMF rather than CO 2 . The control experiments and the in situ high-pressure FT-IR spectra demonstrated that the formation of the carbamate salt of cyclohexylammonium cyclohexylcarbamate ( A ) derived from the reaction of CO 2 with cyclohexylamine was the driving force for this reaction. Accordingly, the mechanism of CO 2 -catalyed N -formylation of aliphatic amines with DMF was proposed, involving the formation of carbamate salt intermediate with enhanced nucleophilicity in anion in favor of the attack on carbonyl-group of DMF.
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JOURNAL OF MEMBRANE SCIENCE
·
2018
·
IF 6.578
Nanjun Chen,Chuanrui Lu,Yunxi Li,Chuan Long,Hong Zhu
Herein, for realizing the high efficiency and long lifetime of hydroxide exchange membranes (HEMs) for alkaline membrane fuel cell (AMFC) applications, a series of robust poly(biphenyl piperidinium) (PBP)/6-azaspiro[5.5] undecane (ASU)-functionalized polyphenyl ether (ASU-PPO) membranes were prepared by a crosslinked strategy. Crosslinked PBP-ASU-PPO membrane combines the advantage of PBP and ASU-PPO membranes as well as addresses the problem of high water uptake of PBP and the insufficient film-forming property of ASU-PPO. As expected, these crosslinked PBP-ASU-PPO membranes exhibit commendably comprehensive performances, such as good ion conductivity, durability, and mechanical properties . The crosslinked PBP-ASU-PPO membrane reaches a maximum OH − conductivity of 128 mS/cm at 80 °C, accompanying with a 15.7% membrane swelling. Besides, only 13.6% degradation in Cl − conductivity was observed in PBP-ASU-PPO after alkaline treatment in 1 M NaOH at 80 °C for 2000 h. Besides, the selected PBP-ASU-PPO membrane achieves a maximum power density of 324 mW/cm 2 at current density of 750 mA/cm 2 .
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CHEMISTRY-A EUROPEAN JOURNAL
·
2017
·Vol. 23
·期 58
·14597-14603
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IF 5.317
Xinghua Chen,Fei He,Yanfei Shen,Yiran Yang,Hao Mei,Songqin Liu,Toshiyuki Mori,Yuanjian Zhang
Graphical Interface effect : A study into the intrinsic role of carbon supports for Fe-N/C alternatives to Pt/C catalysts for oxygen reduction in fuel cells revealed that when immobilized on suitable support, the Fe−N/C demonstrated an improved mass J K that was comparable to that of Pt/C and higher than most reported M−N/C catalysts (see scheme). The mass kinetic current density (mass J K ) of most extensively reported M−N/C catalysts (M represents non-precious metal elements such as Fe, Co, and Cu), a potential alternative to noble metal catalysts in fuel cells, is poorer than that of commercial Pt/C. Thus, deep understanding of the intrinsic roles of carbon supports may contribute to the development of M−N/C catalysts from a practical point of view. Herein, the routinely used carbon supports, i.e. carbon black (CB) and carbon nanotubes (CNT) that have different morphology and crystallinity, were investigated to uncover the factors that affected the mass J K of Fe−N/C in electrocatalytic oxygen reduction. When immobilized on CB, the ionic liquids-derived Fe−N/C exhibited an enhanced mass J K (4.45 A g −1 at 0.80 V vs. RHE) by a factor of 2.14 times, comparable to that of Pt/C (5.79 A g −1 ) and higher than most reported M−N/C catalysts to our best knowledge. In contrast, the CNT support system showed no improvement. It was revealed that a compatible interface between the Fe−N/C precursors and the carbon supports was vital to ensure in-situ growth of a uniform catalyst layer on the supports during pyrolysis. This subsequently promotes the mass J K by exposing more embedded active sites and introducing favorable slit pores for effective mass-diffusion. This work would be promising to address the long-term overlooked challenge of the low mass J K of M−N/C catalysts in replacing noble-metal catalysts for practical fuel cell applications.
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PubMed
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Catalysts
·
2023
·Vol. 14
·期 1
·23
·
IF 3.9
Zi-Han Zhang,An-Qi Wang,Bao-Di Ma,Yi Xu
The effective synthesis ofN-benzyl cyclo-tertiary amines using imine reductase, key components in natural products and pharmaceutical synthesis, is a green approach. Traditional methods faced challenges with enzyme activity and selectivity. This study focused on enhancingMesorhizobiumimine reductase (MesIRED) for betterN-benzyl cyclo-tertiary amine production. Through alanine scanning and consensus mutation, 12 single-siteMesIRED mutants were identified from 23 candidates, showing improved conversion ofN-benzylpyrrolidine andN-benzylpiperidine. Notably, mutants from I177, V212, I213, and A241 significantly boosted conversions. The best-performing mutant forN-benzylpyrrolidine,MesIREDV212A/I213V(M1), increased conversion from 23.7% to 74.3%. ForN-benzylpiperidine,MesIREDV212A/I177A/A241I(M2) enhanced conversion from 22.8% to 66.8%. Tunnel analysis revealed M1 and M2 have more efficient tunnels for larger product movement compared to wild-typeMesIRED. Using recombinantE. colicoexpressingMesIRED and glucose dehydrogenase (GDH), high conversions were achieved: 75.1% forN-benzylpyrrolidine (M1) and 88.8% forN-benzylpiperidine (M2). A preparative experiment resulted in 86.2% conversion and 60.2% yield forN-benzylpiperidine. This research offers an efficient method for engineering IRED, significantly improving conversion and selectivity forN-benzyl cyclo-tertiary amines, aiding drug synthesis and providing insights into rational design of other enzymes.Keywords:imine reductase;N-benzyl cyclo-tertiary amines;alanine scanning;consensus mutation;whole-cell biocatalysis;coexpression
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JOURNAL OF COORDINATION CHEMISTRY
·
2025
·
IF 2.1
Xiaoling Luo,Zheng Liu,Xiaoqi Lan,Pintian Zou,Xiangfei Kong,Guo-Cheng Han
We study the non-covalent interactions within complexes and characterize the structure and properties of N-heterocyclic dicarboxylic acid rare earth complexes. The chelating ligand 2,2′-bipyridine-6,6′-dicarboxylic acid (H2bpdc) was reacted with neodymium nitrate hexahydrate and dysprosium nitrate pentahydrate in a solvothermal reaction to produce {[Nd(bpdc)(HCOO)(H2O)2]·H2O}n (A) and [Dy2(bpdc)3(H2O)2(DMF)]·3H2O (B), respectively. Single crystal X-ray diffraction characterization reveals that A is a metal organic framework, with the rare earth center adopting a nine-coordinated tricapped trigonal prism. In contrast, B forms an eight-coordinate triangular dodecahedron. Fluorescence analyses indicate that both A and B have excellent luminescence properties. The thermal stabilities of both complexes were examined using thermogravimetric analysis (TG and DTG), and A has better thermal stability than B.
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ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Juncheng Zheng,Han Song,Yuankun Yang,Haidong Li,Xuemei Luo,Shu Chen
Persulfate (PDS)-based advanced oxidation processes have emerged as promising methods for antibiotic removal, but achieving high catalytic efficiency for tetracycline (TC) degradation remains difficult. The catalytic performance of FeGCB-N in PDS activation depended on Fe content and pyrolysis temperature, with defect density and intermetallic compound formation largely determined by the pyrolysis temperature. The optimized Fe 0.2 GCB-N-800 exhibited remarkable PDS activation performance for tetracycline degradation, achieving over 99% removal within 65 min under conditions of 10 mg·L -1 TC, 1 mM PDS, and pH 3. X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FT-IR), Raman spectroscopy and X-ray photoelectron spectroscopy (XPS) collectively indicate that surface oxygen-containing functional groups, defect sites, and intermetallic Fe compounds provide active sites for PDS activation by FeGCB. Electron paramagnetic resonance (EPR) and quenching results demonstrated that superoxide radicals (O 2 •- ) and sulfate radicals (SO 4 •− ) were the primary reactive species in TC degradation. Density functional theory (DFT) calculations indicate that Fe-N is the key active site for PDS activation. Based on DFT results and liquid chromatography-mass spectrometry (LC-MS) analysis, potential degradation pathways for tetracycline (TC) are proposed. ECOSAR toxicity assessment showed that the O 2 •- -mediated pathway would generate fewer toxic byproducts. This work offers an effective approach to design environment friendly catalysts from algae biomass for treating wastewater.
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PubMed
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
·
2025
·
IF 5.2
Jiaqi Luo,Yingchen Wang,Qiutong Zhang,Wenhao Yan,Yimin Jia,Mingting Yuan,Qiushuo Yu,Xinyue Zhai,Yuan Zou
N -phenylanthranilic acid (NPAA) is weakly acidic compound that exhibits both excited-state intramolecular proton transfer (ESIPT) and aggregation-induced emission (AIE) characteristics. The molecular structure was confirmed, and its optical behavior was rationalized through a combined approach of quantum chemical calculations and experimental studies. At low concentrations in various solvents, NPAA exhibits dual emission, indicative of an ESIPT process. At higher concentrations, self-association leads to the formation of dimers, resulting in a single emission peak in the fluorescence spectrum. The emission intensity significantly increases with an increasing water fraction in methanol/H 2 O mixtures, demonstrating typical AIE behavior. Additionally, NPAA exhibits time-dependent enhancement of blue-shifted emission and pH-dependent fluorescence responses. Upon adding a large amount of water to the methanol solution (up to about 70 % water fraction), the mixture shows a gradual enhancement accompanied by a blue shift in fluorescence emission. Under alkaline conditions, the carboxyl group becomes negatively charged, which increases intermolecular electrostatic repulsion and weakens hydrogen bonding interactions. As a result, molecular aggregation is inhibited, leading to fluorescence quenching. In contrast, under acidic conditions, the molecules aggregate more readily, which enhances fluorescence emission, and the crystal morphology changes from needle-like to sheet-like. NPAA thus exhibits reversible acid-base responsive fluorescence switching behavior. Furthermore, NPAA films enable reversible fluorescence switching under acid/base vapor stimuli, demonstrating its potential in vapor-responsive luminescent sensing.
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Journal of Materials Chemistry B
·
2015
·Vol. 3
·期 36
·7203-7212
·
IF 4.726
Qiaohua Qiu,Tao Liu,Zhihui Li,Xinbo Ding
Silica–polymer antimicrobial composites with a core–shell nanostructure are often prepared through a polymeric process. However, it is difficult to control the polymerization degree of the polymers to give a uniform size distribution. In this article, we present a facile approach to produce antimicrobial silica@polyacrylamide (SiO2@PAM) core–shell nanoparticles, which were synthesized via an electrostatic self-assembly method using acyclic N-halamine polymeric polyacrylamide. The morphologies and structures of these as-prepared nanoparticles were characterized by different techniques. And their antibacterial performance against both Gram-positive bacteria and Gram-negative bacteria was also evaluated. Based on the preliminary results, these core–shell nanosized spheres were made of an outer polymer shell which decorated the inner SiO2 core, showing the encapsulation of silica nanoparticles with PAM polymers. After chlorination, the resultant nanosized particles displayed a powerful and stable bactericidal capability toward both of the two model bacterial species. Bactericidal assessment further suggested a coordinated effect of the well-known antibacterial performance of N-halamines and the flocculation of PAM on the antibacterial behavior. The in vitro cytotoxicity of the prepared nanoparticles with varying concentrations was studied using mouse fibroblast cells (L929). The CCK-8 assay revealed that the SiO2@PAM composites possessed a non-cytotoxic and favorable response to the seeded cells in vitro. These results indicate the suitability of the SiO2@PAM composite particles for controlling biocidal activity, demonstrating their potential applications in deactivating bacteria or even disease control.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Md Manik Mian,Guijian Liu,Biao Fu,Yu Song
Sewage sludge (SS), the inevitable byproduct of wastewater treatment plants, is facing numerous challenges of environmentally safe and cost-effective disposal. Thus, exploration of efficient SS valorization technique is highly desired. In this study, a sludge derived carbon-supported MnO x as a catalyst (ASMn-Nb) was synthesized through NH 4 OH activation and pyrolysis (800 °C) to enhance peroxymonosulfate (PMS) decomposition and subsequent degradation of acid orange 7 and rhodamine B. The sample characterization indicated that MnCl 2 conditioning produces mixed valent Mn oxides on ASMn-Nb, while NH 4 OH activation significantly enhances N-heteroatoms, surface area, and microporosity. The as-synthesized hybrid catalyst exhibited excellent PMS decomposition ability in a wide range of pH, which enhances AO7 removal efficiency 16%–100% in 40 min compared with that treated with raw sludge biochar. Moreover, the catalyst is recyclable, chemically stable, and produce negligible metal leaching during catalysis. Further investigation of catalytic mechanisms revealed that both radicle and non-radicle processes governing PMS decomposition, whereas mediated electron transfer as the primary and 1 O 2 , SO 4 − , and OH radicals induced catalysis as the secondary mechanisms of PMS activation and subsequent AO7 degradation. Finally, a probable mechanism of PMS decomposition over ASMn-Nb and AO7 degradation path is proposed. This study concurrently provides a facile route of improving the catalytic performance of sludge derived-biochar and a probable SS valorization technique.
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Nano Research
·
2021
·Vol. 15
·期 3
·1824-1830
·
IF 8.897
Wang Chao,Li Wen,Wang Xiaodan,Yu Nan,Sun Hongxia,Geng Baoyou
Molybdenum phosphide is a potential hydrogen evolution reaction (HER) catalyst. However, traditional high-temperature phosphating preparation methods are prone to damage of material morphology and agglomeration. Using the carbon skeleton to limit the size and morphology of MoP and to improve the conductivity of the material is an effective method to improve the performance of the catalyst. However, there is a lack of research on the effect of carbon skeleton and MoP composite structure on the catalytic mechanism of HER. We coated ZIF-8 on the surface of MoP nanorods, and obtained open N-doped carbon-coated porous MoP nanorods (N/C/MoP) through carbonization and phosphating. Studies have shown that the ZIF-8 coating effectively limits the size and morphology of the material and avoids agglomeration. Under alkaline conditions, N/C/MoP has a low overpotential of 169 mV for HER at 10 mA/cm 2 , which is 55 mV lower than MoP without a carbon layer. At the same time, its Tafel slope (51.3 mV/dec) is smaller than Pt/C (59.9 mV/dec), and it has good stability. Density functional theory (DFT) studies have shown that under alkaline conditions, there is a synergistic effect between the open N-doped carbon layer and the exposed MoP active surface, which reduces the activation energy of water and improves the catalytic performance of HER. It is worth noting that a tight coating will hinder the exposure of active sites and reduce catalytic activity.
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Nanoscale
·
2019
·Vol. 11
·期 41
·19506-19511
·
IF 6.97
Ying Li,Tong Liu,Wenxiu Yang,Zhijun Zhu,Yanling Zhai,Wenling Gu,Chengzhou Zhu
Non-Pt catalysts with excellent performance regarding the oxygen reduction reaction (ORR) have aroused enormous interest in recent years. Herein, we propose a dual-template method to synthesize a multiscale porous Fe–N–C (FeNC) catalyst. SiO2 and Zn are used as co-templates to produce a multiscale porous structure. Chitosan and glutaraldehyde are used as building blocks to fabricate the frameworks of the hydrogel. After lyophilization and annealing treatments, FeNC aerogel with a multiscale porous structure could be obtained. The as-prepared FeNC catalyst annealed at 900 °C (FeNC-900) exhibits a larger electrochemically active surface area and an improved ORR activity compared to FeNC annealed at other temperatures. FeNC-900 shows a superior ORR performance in comparison with that of commercial Pt/C in terms of the onset potential and half-wave potential, i.e., 0.959 and 0.837 V, which are 28 mV and 10 mV higher than those of Pt/C, respectively. Multiscale porosity is responsible for the outstanding ORR performance of FeNC-900. The electron transfer number of FeNC-900 for the ORR was calculated to be 3.95, which is comparable with that of Pt/C. In addition, the FeNC-900 catalyst possesses an excellent long-term duration and anti-poisoning capacity against methanol crossover. All these results endow the FeNC catalyst with tremendous potential for use in fuel cells.
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