ChemSusChem
·
2015
·Vol. 8
·期 12
·2066-2072
·
IF 7.657
Yehong Wang,Jian Zhang,Jing Liu,Chaofeng Zhang,Zhixin Zhang,Jie Xu,Shutao Xu,Fangjun Wang,Feng Wang
Graphical CO 2 -mediated reactions: CO 2 -mediated metathesis reactions between amines and DMF to synthesize formamides are described. The N -formylation of amines to formamides is achieved by activating amines, not DMF, via a C N and N H bond metathesis reaction. Using this method, primary, secondary, aromatic, and heterocyclic amines as well as diamines can be obtained with good to excellent formamide yields. Herein, we report CO 2 -mediated metathesis reactions between amines and DMF to synthesize formamides. More than 20 amines, including primary, secondary, aromatic, and heterocyclic amines, diamines, and amino acids, are converted to the corresponding formamides with good-to-excellent conversions and selectivities under mild conditions. This strategy employs CO 2 as a mediator to activate the amine under metal-free conditions. The experimental data and in situ NMR and attenuated total reflectance IR spectroscopy measurements support the formation of the N -carbamic acid as an intermediate through the weak acid–base interaction between CO 2 and the amine. The metathesis reaction is driven by the formation of a stable carbamate, and a reaction mechanism is proposed.
研究领域:
有机化学
·
绿色化学
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DOI
PubMed
高影响因子
FUEL
·
2018
·
IF 4.908
Lifeng Zhang,Hao Ying,Shu Yan,Ningning Zhan,Yongsheng Guo,Wenjun Fang
Two kinds of hyperbranched poly(amido amine) (h-PAMAM) with abundant terminal amine groups are synthesized to break the oil-in-water (O/W) emulsions consisting of microdroplets. The demulsification performance of h-PAMAM is systematically evaluated with assistance of UV–vis spectra, micrograph, DLS and SAXS analyses. The demulsifier with 1,3-propanediamine as initiator shows a striking demulsification ability with small dosage (<40 mg/L). The demulsification equilibrium can be obtained within 30 min, and oil removal ratio reaches to 92%, which is ascribed to the highly hyperbranched structure and the adequate molecular weight. The demulsifier molecules with hyperbranched structure easily diffuse to the oil-water interface and reveal a high interfacial activity, which causes film break and coalescence of oil droplets, and consequently leads to high oil removal ratio. The combination of UV–vis spectra, micrograph, DLS and SAXS analyses provides a new approach to monitor demulsification process and comprehend demulsification mechanism. The excellent demulsification performance of h-PAMAM shows a considerable potential applications of this hyperbranched polymer for wastewater treatment and petroleum industry.
研究领域:
化学工程
·
环境科学
·
石油工业
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产品关联
DOI
高影响因子
Polymer Chemistry
·
2024
·
IF 4.1
Hong-Hui Shu,Yun Liu,Sheng-Li Han,Xiuqin Fang,Chang Wang,Cheng-Mei Liu
Biomass-based polyamides (bioPAs) are renewable materials that are viable alternatives to petroleum-based polyamides in the engineering field. However, the attention to designing functional bioPAs with tunable properties has been limited. Herein, by taking furfurylamine as the sole furan source, we first utilized amine-acid oxidative coversion to prepare bisfuranic diacid monomer directly from bisfuranic diamine monomer(amine-first strtegy), it was totally different to castor oil-based acid-first strategy of preparing PA1010. Then the as-prepared multifunctional diamine/diacid monomers underwent polycondensation to obtain all-furan based bioPAs with or without functinal pendant groups. The properties of bioPAs, incuding glass transition temperatue, degradation character, solubility, etc, can be regulated over a larger range through the design of the spacer structure between two furan rings on diamine monomers. Charged bioPAs with cationic or anionic groups were further developed by postpolymerization modification. The oppositely charged bioPAs, sharing an identical main chain structure but different pendent groups, formed porous polyelectrolyte complexes owing to their rigid main chain. Therefore, this research provides a novel strategy for preparing both functional and engineering furan-based bioPAs.
研究领域:
材料科学
·
高分子化学
·
可持续材料
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产品关联
DOI
高影响因子
CRYSTAL GROWTH & DESIGN
·
2020
·
IF 4.089
H. Liu,X. Yang,S. Cao,F. Yu,S. Long,J. Chen,M. Zhang,S. Parkin,T. Li,Z. Yang
A series of N-phenyl-2-hydroxynicotinanilides (PHNAs) have been synthesized, and their crystal structures have been investigated. The identity of these compounds is revealed to be the tautomer of PHNAs, i.e., 2-oxo-1,2-dihydropyridine-3-carboxylic acid phenylamides, compounds with both amide and lactam functionalities. Among these compounds, those with no or negligible steric hindrance take a near planar conformation and form lactam–lactam dimers, not the widely observed amide NH···O═C hydrogen bond chains, while those with steric hindrance take a twisted conformation and form an amide NH···O═C (lactam) hydrogen bond. A succinct theoretic study combining conformational analysis and molecular electrostatic potential surfaces (MEPS) survey provided a reasonable explanation of the formation of these two different hydrogen bond motifs.
研究领域:
化学
·
晶体学
·
理论计算
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产品关联
DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Shaoliang Zhu,Bingtao Zhao,Yaxin Su
High-efficiency and cost-effective adsorbents are crucial to dry capture of carbon dioxide (CO 2 ). The polyethyleneimine (PEI) was co-impregnated with tetraethylenepentamine (TEPA) on γ-alumina (Al 2 O 3 ) to synthesize the adsorbent and enhance the capture process. The influence of amine loading and operating parameters on CO 2 adsorption was investigated, and the process parameters were modeled. The results depict that the optimal loading is 50 % when functionalized either PEI or TEPA individually, which is 3.7 and 4.6 times higher than γ–Al 2 O 3 . The CO 2 capacity of γ–Al 2 O 3 functionalized with multiple amines (30 %PEI+20 %TEPA) is 2.65 mmol/g, due to the synergies of the two amines to increase the chance of CO 2 binding to the sites. Regeneration performance illustrates that the adsorbent remains at 90.2 % of the initial capacity after seven tests. The maximal capacity of 2.70 mmol/g occurs at 70 °C. Modeling results indicate the kinetics can be evaluated by the Avrami model (R 2 > 0.990) with the activation energy of 5.65 kJ/mol. The process is controlled by physical–chemical adsorption, influenced by intraparticle diffusion, as described by the deactivation model. Finally, a comparison and assessment were conducted for their techno-economic performances, and the pathway to applications was also proposed in engineering practice.
研究领域:
化学工程
·
环境科学
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产品关联
DOI
高影响因子
Journal of Water Process Engineering
·
2024
·
IF 6.3
Jian Dong,Yi Wang,Liangliang Dong,Tatsuo Kaneko,Weifu Dong,Dongjian Shi,Mingqing Chen
To address the membrane challenges such as the trade-off effect between water permeance and separation selectivity, development of a desirable nanofiltration membrane structure is crucial. And, it is important to design a positively charged surface to enhance charge repulsion force between membrane surface and ions due to lithium (Li) extraction problem as the close hydration diameter of magnesium (Mg) and lithium ions. Herein, a strategy that involves regulating membrane structure to create a loose and dense double-layer structure via bi-directional interfacial polymerization has been proposed to form selectivity-enhanced nanofiltration membranes for Li + /Mg 2+ separation. The incorporation of dopamine (DA) and trimesoyl chloride (TMC) in first loose layer could improve the membrane stability, while the amine groups from polyethyleneimine (PEI) or polyvinylamine (PVAm) in the second dense layer surface, provided by rich amine polymers, could improve the rejection of divalent magnesium ion. The as-fabricated membrane DA-TMC-PEI shows enhanced permeance (around 15.4 L m −2 h −1 bar −1 ) and the membrane DA-TMC-PVAm demonstrates outstanding ion selectivity with Li + /Mg 2+ separation factor of 30. Moreover, the DA-TMC-PEI and DA-TMC-PVAm membranes could efficiently purify the ratio of Mg 2+ /Li + solution from 50 to 0.43. We believe the strategy could provide a promising potential in lithium extraction.
研究领域:
材料科学
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环境工程
·
化学工程
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产品关联
DOI
高影响因子
DYES AND PIGMENTS
·
2020
·
IF 4.613
Beitong Zhu,Lirong Jiang,Tianhong Chen,Guang-Ming Bao,Lintao Zeng,Xichao Hu,Hou-Qun Yuan
Biogenic primary diamines are a family of critical food spoilage biomarkers. To maintain food safety, it is necessary to implement highly efficient detection methods to monitor the levels of biogenic primary diamines in edible products. In this study, we report a 7-diethylaminocoumarin derivative, CMA-Cl, as a colorimetric and fluorescence lighting-up probe for detecting critical biogenic primary diamines including cadaverine and putrescine. The CMA-Cl probe underwent a nucleophilic substitution and condensation reaction with biogenic primary diamines, generating highly emissive compounds, which displayed strong emission at 475 nm with a fluorescence quantum yield of 36.4%. The CMA-Cl probe showed colorimetric and fluorescence dual-response towards biogenic primary amines with a significant linear relationship, good selectivity, and low limit of detection (209 nM). The probe demonstrated a good recovery (97–122%) for the determination of a typical biogenic primary diamine cadaverine during the spoilage of fish. Furthermore, CMA-Cl -loaded paper was fabricated for the real-time visual detection of a typical biogenic primary diamine cadaverine in fish samples based on distinct changes in color and fluorescence.
研究领域:
食品安全
·
分析化学
·
生物化学
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DOI
高影响因子
Journal of Materials Chemistry C
·
2022
·Vol. 10
·期 45
·17225-17235
·
IF 8.067
Man Liu,Yiheng Song,Hongmei Qin,Ziwei Li,Yuheng Fu,Chuanxi Xiong,Feihua Liu
Polymers with both high dielectric breakdown strength and high dielectric constant are vital for a large number of applications. However, most polymer or polymer composites suffer from the problem of deteriorated breakdown strength caused either by undesired submicron voids during film processing or the addition of high dielectric constant filler. In this work, we present a facile blending strategy to fabricate polyamide-imide (PAI)/polyimide (PI) alloy. The strong interchain hydrogen bonds and electrostatic force of the PAI/PI alloy increase chain packing density and decrease possible corresponding imperfect points. The intermolecular forces are simulated and calculated via Materials Studio. It is found that the PAI/PI alloy with 50 wt% PAI possesses the strongest intermolecular forces, which is consistent with the experimental results. The PAI/PI alloy with 50 wt% PAI exhibits enhanced dielectric properties, such as 54.3% improvement in breakdown strength, 68.8% enhancement in dielectric constant and suppressed dielectric loss compared with pristine PI, leading to a high discharged energy density of 5.84 J cm−3 with an efficiency of 91.8% at 545 MV m−1. The excellent performance of the PAI/PI alloy can be attributed to the polar groups in PAI that promote the dielectric constant, strong hydrogen bonds and electrostatic force between the molecule chains in the blend that contribute to the greatly enhanced breakdown strength. This novel molecular engineering strategy is an effective way to fabricate high-performance dielectric polymers for film capacitor applications.
研究领域:
材料科学
·
高分子化学
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产品关联
DOI
高影响因子
LANGMUIR
·
2023
·
IF 3.9
Ze-Lin Qiu,Wen-Han Yu,Wu-Shang Yang,Tong Sun,Zi-Hao Zhao,Qian-Wei Su,Bao-Ku Zhu
High-efficiency dye desalination is crucial in the textile industry, considering its importance for human health, safe aquatic ecological systems, and resource recovery. In order to solve the problem of effective separation of univalent salt and ionic dye under the condition of high salt, ionic hyperbranched poly(amido-amine) (HBPs) were synthesized based on a simple and scalable one-step polycondensation method and then incorporated into the polyamide (PA) selective layers to construct charged nanochannels through interfacial polymerization (IP) on the surface of a polyvinyl chloride ultrafiltration (PVC-UF) hollow fiber membrane. Both the internal nanopores of HBPs (internal nanochannels) and the interfacial voids between HBPs and the PA matrix (external nanochannels) can be regarded as a fast water molecule transport pathway, while the terminal ionic groups of ionic HBPs endow the nanochannels with charge characteristics for improving ionic dye/salt selectivities. The permeate fluxes and dye/salt selectivities of HBP-TAC/PIP (57.3 L m–2 h–1 and rhodamine B (RB)/NaCl selectivity of 224.0) and HBP-PS/PIP (63.7 L m–2 h–1 and lemon yellow (LY)/NaCl selectivity of 664.0) membranes under 0.4 MPa operation pressure are much higher than PIP-only and HBP-NH2/PIP membranes. At the same time, this project also studied the membrane desalination process in a simulated high-salinity dye/salt mixture system to provide a theoretical basis and technical support for the actual dye desalination process.
研究领域:
材料科学
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环境工程
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Xiaoyu Li,Xueqi Zhao,Yao Meng,Haiyang Xue,Jie Chen,Kang Peng
Blending two amines has recently been developed as an efficient strategy to improve the post-combustion CO 2 capture performance of amine-functionalized mesoporous materials. The mixed two amine species of polyethyleneimine (PEI) and diethanolamine (DEA) can help to overcome the problems of intrinsic large viscosity, easy aggregation and low amine efficiency of the polyamine. In this study, a novel additive promoted supported mixed amines on mesoporous silica were successfully synthesized via a facile and efficient wet impregnation route. The adsorption performance of PEI and DEA individually loaded onto Al-MCM-41 was tested at 75 °C in a flow of 60 vol% CO 2 /40 vol% N 2 , leading to the identification of an optimal mixed amine loading of 50 %. The supported mixed amines system was further evaluated based on amine efficiency, adsorption capacity, kinetics and stability. The optimal adsorbent loaded with 30 wt% PEI and 20 wt% DEA exhibits a maximum CO 2 uptake of 3.53 mmol/g at 75 °C and stable cyclic stability with an average 1.93 % decay per cycle, due to the synergistic effect of both amines. The DEA with hydroxyl groups was introduced into PEI and co-impregnated within mesoporous silica can overcome the poor mass transfer of PEI, the limited stability of DEA and low adsorption capacity of Al-MCM-41. The synergistic combination of PEI and DEA is able to provide abundant CO 2 affinity sites and create extra CO 2 transfer pathways for effectively reducing the internal CO 2 diffusion resistance, by which the diffusion limitation of CO 2 in the deeper PEI films can be alleviated due to the interactions between PEI and DEA. As a result, the final mixed amine-functionalized adsorbents have excellent cyclic CO 2 uptake capacity, rapid kinetics and stability. This approach holds significant promise for environmentally friendly, cost-efficient, and large-scale applications in CO 2 capture and separation.
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
·
2024
·
IF 6.2
Rongfang Yang,Jiaxin Zhang,Xiumei Xing,Shiyuan Zhong,Wenxue Li,Lixian Wen,Yuwei Zhang,Hongwei Zhou,Shen Chen,Wen Chen,Yongmei Xiao,Liping Chen
Benzene exposure has been linked to various adverse health effects. However, the effective strategy for prevention or treatment of benzene-induced hematotoxicity remains unsolved. We previously administrated hepatocyte-specific deletion of Ppp2r1a gene (encoding PP2A Aα subunit) mice with benzene via inhalation for 28 days, and found homozygote (HO) mice exhibited alleviative hematotoxicity compared with wild type (WT) mice. Here, we integrate untargeted metabolomics and transcriptomics data to identify the key metabolic pathways and metabolites attenuating benzene-induced hematotoxicity. Metabolomics analysis revealed the perturbation of nicotinate and nicotinamide metabolism, as well as taurine and hypotaurine metabolism pathways, were implicated in regulating benzene-induced hematotoxicity. Meanwhile, transcriptome analysis showed that immune-, inflammation-, and metabolism-related pathways were obviously disturbed in WT mice groups upon benzene exposure, while sirtuin signaling pathway, associated with nicotinate and nicotinamide metabolism, was activated in HO mice groups. Notably, combined metabolomics and transcriptomics analysis further confirmed the involvement of nicotinate and nicotinamide metabolism, taurine and hypotaurine metabolism pathways in relieving benzene-induced hematotoxicity. Specific metabolites, including 1-methylnicotinamide (MNA), nicotinamide (NA), β-nicotinamide mononucleotides (NMN), and taurine were identified as the potential metabolites alleviating benzene-induced adverse effects. In vitro experiments demonstrated the protective effect of MNA and NA against 1,4-benzoquinone (1,4-BQ)-caused cytotoxicity in HL-60 cells. In vivo , MNA supplementation in drinking water could effectively restore the decline in white blood cell (WBC), lymphocyte (LYMPH), and reticulocyte (RET) counts, also mitigate oxidative damage and genotoxicity in response to benzene exposure. These observations highlight the potential of MNA supplementation as a strategy for preventing benzene-caused hematotoxicity.
研究领域:
毒理学
·
代谢组学
·
分子生物学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Ting Huang,Sheng Cao,Dan Luo,Nan Zhang,Yan-zhou Lei,Yong Wang
Melamine foam (MF) is a widely used commercial product and exhibits wide applications in many fields ranging from building, transportation to daily chemical product. Recent researches confirm that the special three-dimensional (3D) framework structure of MF can be an ideal substrate to prepare functional materials. In this work, the water-soluble polyethylenimine (PEI) was grafted onto the framework of MF to develop the water purification material toward heavy metal ions removal. The grafting of PEI on MF was achieved with the aids of polydopamine (PDA) coating and epoxy chloropropane (ECH) cross-linking successively. The 3D framework of MF could be well reserved and PEI was homogeneously grafted onto the framework surface. The adsorption capacity of the adsorbent was dependent upon the molecular wight of PEI. Lower PEI molecular weight endowed the adsorbent with better adsorption ability. The maximum adsorption capacity reached 328.95 mg/g, and the adsorbent exhibited extremely high adsorption stability with increasing cycling measurement numbers. Further results showed that the adsorbent also exhibited high reduction ability and induced about 62.5% toxic Cr(VI) to be reduced. This work confirms that the PEI-modified MF sample is a promising adsorbent in the removal of heavy metal ions and it can be used in wastewater treatment .
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
DOI
PubMed
高影响因子