CHEMICAL COMMUNICATIONS
·
2011
·Vol. 48
·期 14
·2024-2026
·
IF 5.787
Jian Gao,Qing-Wen Song,Liang-Nian He,Zhen-Zhen Yang,Xiao-Yong Dou
An iron(III)-catalyzed three-component coupling reaction of alkynes, CH2Cl2 and amines was developed for facile synthesis of propargylamines. Preliminary mechanism investigation using in situFT-IR reveals that the crucial Fe-acetylide intermediate could be formed through C–H bond activation of alkynes thanks to cooperative effect of FeCl3 and 1,1,3,3-tetramethylguanidine.
研究领域:
有机化学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Polymer Chemistry
·
2021
·Vol. 12
·期 46
·6694-6704
·
IF 5.582
Yu Liu,Weichen Sheng,Ren Yin,Kan Zhang
Aniline is a very common amine source for benzoxazine synthesis, but it generally results in relatively high ring-opening polymerization temperatures. The exploration of alternative amine sources to lower the polymerization temperature of benzoxazine resins is a prerequisite for further development of high performance polybenzoxazines. In this work, three propargyl-containing benzoxazine monomers with different numbers of oxazine rings (PH-pa, BA-pa and TH-pa) have been synthesized using phenol/bisphenol-A/1,1,1-tris(4-hydroxyphenyl)ethane, propargylamine, and paraformaldehyde as the starting materials. The structures of these benzoxazines are characterized using NMR, FT-IR and HR-MS spectra, which indicate the successful incorporation of the reactive oxazine ring and the propargyl group into the molecular structure of each monomer. In addition, the polymerization behavior of each benzoxazine has been monitored by in situ FT-IR spectroscopy and differential scanning calorimetry (DSC), which shows that each resin can be completely polymerized through complex polymerization mechanisms including the ring-opening polymerization of the oxazine ring and additional ethynyl polymerization. Moreover, the thermal stability and the flammability of the resulting thermosets have been investigated by thermogravimetric analysis (TGA) and micro-scale combustion calorimetry (MCC), respectively. Notably, the thermoset derived from TH-pa exhibits the highest thermal stability with a peak degradation temperature of 418 °C and a char yield value of 50.2% at 800 °C in nitrogen. It also exhibits the lowest heat release capacity (87.0 J g−1 K−1) and total heat release value (17.4 kJ g−1) among the newly obtained polybenzoxazines.
研究领域:
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2025
·
IF 6.5
Lingfang Kong,Yi Liu,Zhonggao Zhou,Zhichao He,Yun Bai,Guohai Xu,Yunxiang Pan,Hongyu Zhen,Yiwang Chen
The conversion of carbon dioxide (CO 2 ) and propargylamines to 2-oxazolidinones is an essential reaction in industry, but efficiently activating both feedstocks remains a huge challenge for majority of catalysts. Herein, we developed a long-term stable copper catalyst, co-coordinated with sugar acetates (acetylglucose, AcGlu) and 2-methyl-imidazolium (Im-Cu A ). This catalyst features multi-active site, enabling it to efficiently capture and activate CO 2 , activate propargylamines, and stabilize the catalyst species simultaneously. As expected, 2-oxazolidinone was synthesized by this cyclization reaction with an exciting turnover frequency of 880 h −1 , which is around 180 times higher than that of CuCl 2 . Moreover, the catalytic activity of Im-Cu A did not decrease even after 20 replicates, which is exceptionally rare for homogeneous catalysts. Density functional theory calculations indicate that the electron-donating AcGlu and 2-methyl-imidazolium units facilitate electrons transport from Im-Cu A to CO 2 . Moreover, the high electron density of AcGlu and 2-methyl-imidazolium groups is believed to play a crucial role in the long-term stability across various temperatures and excellent catalytic performance of Im-Cu A . This represents a significant advancement in the development of a highly stable copper catalyst with multi-active site that effectively activates all reaction substrates. This strategy could improve the development of metal catalysts with sustained superior performance for CO 2 conversion.
研究领域:
化学催化
·
材料科学
·
环境科学
✓ 已验证
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2016
·
IF 5.267
Yuling Zhao,Jikuan Qiu,Li Tian,Zhiyong Li,Maohong Fan,Jianji Wang
Carbon dioxide (CO2) is an abundant and renewable feedstock for the production of high-value chemicals. Herein, CuI and 1,8-diazabicyclo[5.4.0]undec-7-ene (DBU) were employed as an efficient catalyst system to synthesize 2-oxazolidinones through the coupling reaction of CO2 and propargylic amines. It was found that this cost-competitive catalyst system could efficiently catalyze the reaction within only 4 h at atmospheric pressure CO2, and a wide range of substrates were suitable for this reaction. Various target products were obtained in excellent yields. Furthermore, the catalytic mechanism of the CuI/DBU system was investigated by using density functional theory. It was shown that copper(I) and DBU played synergistic roles in activating both the C≡C triple bond and the amino group of propargylic amines in the reaction.
研究领域:
有机化学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Weibo Huang,Yan Wang,Linze Lv,Yueyue Wang,Xiang Li,Honghe Zheng
Silicon (Si) is deemed to be the next-generation lithium-ion battery anode. However, on account of the poor electronic conductivity of Si materials and the instability of the solid electrolyte interphase layer, the electrochemical performance of Si anodes is far from reaching the application level. In this work, a multifunctional poly(propargylamine) (PPA) interlayer is constructed on the Si surface via a simple in situ polymerization method. Benefiting from the electronic conductivity, ionic conductivity, robust interphase interactions for hydrogen bonding, and stability of multifunctional PPA, the optimized Si@PPA-7% electrode shows improved lithium storage capability. A high capacity of 1316.3 mAh g–1 is retained after 500 cycles at 2.1 A g–1, and 2370.3 mAh g–1 can be delivered at 42 A g–1, which are in stark contrast to the unmodified Si electrode. Furthermore, the rate and cycle capabilities of the LiFePO4//Si@PPA-7% full cell are also obviously better than those of LiFePO4//Si.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
PubMed
高影响因子
MICROCHIMICA ACTA
·
2014
·Vol. 181
·期 15
·1981-1989
·
IF 3.719
He Linghao,Zhang Yuanchang,Liu Shunli,Fang Shaoming,Zhang Zhihong
We report on a novel graphene-based nanoarchitecture modified with plasma-polymerized propargylamine (G-PpPG) and its application in electrochemical sensors for DNA. Films of G-PpPG were characterized by X-ray photoelectron spectroscopy and electrochemical impedance spectroscopy. The presence of graphene enhances the electrochemical activity of the films, and the high density of amino groups (deposited at a low plasma input power) on their surface assists in the immobilization of probe DNA on the water-swollen polymeric network. By contrast, the degree of hybridization of the total complementary target DNA to the probe DNA remains unchanged when G-PpPG nanofilms prepared at higher input power. No substantial non-specific adsorption of totally mismatched target DNA on the polymer films is observed because of the complete coverage of the probe DNA. The detection limit for total complementary target DNA is approximately 1.84 nmol · L −1 . The dynamic range extends from 0.1 to 1,000 nmol · L −1 . The new nanocomposite may also be used to immobilize other probe DNA sequences, and this makes the approach potentially applicable to the detection of other oligomers.
Preparing the DNA sensor made from the graphene-based nanoarchitecture modified by using PpPG (G-PpPG) includes the following processes: (a) Modifying the Au electrode with the graphene nanosheet, (b) depositing the PpPG film onto the Au electrode coated with graphene, (c) immobilizing the probe DNA onto the G-PpPG film, and (d) hybridizing the MM0 target with the G-PpPG film immobilized with P1
研究领域:
生物传感
·
材料科学
·
分子生物学
✓ 已验证
产品关联
DOI
高影响因子
PLASMA CHEMISTRY AND PLASMA PROCESSING
·
2016
·Vol. 36
·期 4
·1051-1065
·
IF 1.811
Peng D. L.,Ji H. F.,Dong X. D.,Tian J. F.,Wang M. H.,He L. H.,Zhang Z. Z.,Fang S. M.
In this study, a nanocomposite consisting of three-dimensional reduced graphene oxide (3D-rGO) and plasma-polymerized propargylamine (3D-rGO@PpPG) was prepared and used as a highly sensitive and selective DNA sensor for detecting Hg 2+ . Given the high density of amino groups in the resultant 3D-rGO@PpPG nanocomposite, thymine-rich and Hg 2+ -targeted DNA was preferentially immobilized on the fabricated sensor surface via the strong electrostatic interaction between DNA strands and the amino-functionalized nanocomposites, followed by detecting Hg 2+ through T–Hg 2+ –T coordination chemistry between DNA and Hg 2+ . The results of electrochemical measurements revealed that the anchored amount of DNA strands anchored on the 3D-rGO@PpPG nanofilm surface affects the determination of Hg 2+ in aqueous solution. It showed high sensitivity and selectivity toward Hg 2+ within concentrations ranging from 0.1 to 200 nM and displayed a low detection limit of 0.02 nM. The new strategy proposed also provides high selectivity of Hg 2+ against other interfering metal ions, good stability, and repeatability. The excellent applicability of the developed sensor confirms the potential use of plasma-modified nanofilms for the detection of heavy metal ions in real environmental samples and water.
研究领域:
環境科學
·
分析化學
·
納米技術
·
生物技術
✓ 已验证
产品关联
DOI
高影响因子
MACROMOLECULAR CHEMISTRY AND PHYSICS
·
2020
·Vol. 221
·期 18
·2000157
·
IF 2.335
Ming Gao,Hang Lu,Rong-Hao Song,Lin Ye,Ai-Ying Zhang,Zeng-Guo Feng
To highlight whether γ-cyclodextrins (CDs) facilitate propargylamine monosubstituted β-CDs (PA-β-CDs) as end stoppers to get threaded onto a distal azide terminated poly(2-hydroxyethylmethacrylate) (PHEMA) homopolymer (PH-46-2N 3 ) to create linear and hyperbranched polyrotaxanes (PRs) via the in situ copper-catalyzed azide/alkyne cycloaddition (CuAAC), PH-46-2N 3 is self-assembled with a varying amount of γ-CDs in water and then subjected the CuAAC with PA-β-CDs to end-cap the resulting γ-CD-PHEMA polypseudorotaxanes (PPRs) into the γ-CD-PHEMA PRs. It demonstrates that γ-CDs cannot promote PA-β-CDs to be entrapped on the PHEMA chain most likely due to their different cavity size and molecular framework and linear PRs are always formed with up to 29% γ-CD coverage ratio along the PHEMA axis thereof.
研究领域:
高分子化学
·
超分子化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
POLYMER
·
2023
·
IF 4.6
Ming Gao,Chun-jiang He,Xue Geng,Lin Ye,Ai-ying Zhang,Zeng-guo Feng
When γ-CDs were self-assembled with a distal 2-chloropropionyl terminated poly (ethylene glycol) (PEG-2Cl) in aqueous solution, two distinct polypseudorotaxanes (PPRs), a single stranded one and a double stranded one were identified from the upper clear solution and the lower precipitates, respectively. Moreover, if the chlorine groups in PEG-2Cl were converted into the azido groups to give a bifunctional azido terminated PEG (PEG-2N 3 ) and then subjected to the inclusion complexation with γ-CDs, two similar double stranded PPRs were lyophilized from the upper and lower layer products. To probe whether the parallel or bent double stranded PPRs were created from the self-assembly of γ-CDs with PEG-2N 3 , the in situ copper-catalyzed azide/alkyne cycloaddition (CuAAC) was conducted to transform the resulting PPRs into the PRs using propargylamine monosubstituted β-CDs (PA-β-CDs) as bulky stoppers. After thorough purification, both the upper and lower layer products lyophilized therefrom were revealed the same parallel double stranded PRs by spectral and thermal analyses.
研究领域:
材料科学
·
聚合物化学
·
超分子化学
✓ 已验证
产品关联
DOI
高影响因子
MICROCHIMICA ACTA
·
2015
·Vol. 183
·期 2
·633-642
·
IF 3.741
Fang Shaoming,Dong Xiaodong,Ji Hongfei,Liu Shunli,Yan Fufeng,Peng Donglai,He Linghao,Wang Minghua,Zhang Zhihong
This article describes an aptasensor for lysozyme that is based on a gold electrode modified with an aptamer-wrapped composite consisting of three-dimensional reduced graphene oxide, cuprous oxide, and plasma-polymerized propargylamine (Cu 2 O@rGO@PpPG) as the sensing layer. The nanocomposite consisting of Cu 2 O@rGO was synthesized by simultaneously reducing GO and Cu(II) ions with glucose and then modified by plasma-enhanced chemical vapor deposition using propargylamine as the monomer gas. The resulting amine-rich nanofilms of Cu 2 O@rGO@PpPG nanocomposite were deposited on a gold electrode. Differential pulse voltammetry and electrochemical impedance spectroscopy show these layers to exhibit a good amperometric response and variation of the charge transfer resistance to lysozyme after aptamer strands had been immobilized on the films via electrostatic interaction between the negatively charged phosphate groups of the aptamer and the positively charged amino groups on the electrode. The sensor, when operated at 0.22 V (vs. Ag/AgCl), can detect lysozyme in the 0.1 nM to 200 nM concentration range with a 0.06 nM limit of detection. In addition, the sensor displays excellent selectivity and repeatability. In our perception, this strategy for preparing aptasensors holds a great potential with respect to the use of plasma-modified nanocomposites in clinical analysis.
An effective aptasensor was constructed using a nanocomposite consisting of three-dimensional reduced graphene oxide, cuprous oxide, and plasma-polymerized propargylamine as the sensitive layer. It exhibits a detection limit of 0.06 nM and an analytical range of 0.1 to 200 nM.
研究领域:
分析化学
·
纳米技术
·
生物传感器
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）