PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2023
·Vol. 25
·期 11
·8050-8063
·
IF 3.3
Luyi Wang,Jianjun Zhao,Jun Chen,Tingting Jiang,Qian Zhang,Shengwen Zhong,Sydorov Dmytro
In this study, phenediamine bridging phthalocyanine-based covalent organic framework materials (CoTAPc-PDA, CoTAPc-BDA and CoTAPc-TDA) with increasingly-widening pore sizes are prepared by reacting cobalt octacarboxylate phthalocyanine with p-phenylenediamine (PDA), benzidine (BDA) and 4,4′′-diamino-p-terphenyl (TDA), respectively. The effects of frame size on the morphology structure and its electrochemical properties were explored. X-ray diffraction (XRD), Brunauer–Emmett–Teller (BET) and transmission electron microscopy (TEM) images show that the pore sizes of the CoTAPc-PDA, CoTAPc-BDA and CoTAPc-TDA are about 1.7 nm, 2.0 nm and 2.3 nm, respectively, which are close to the simulated results after geometric conformation optimization using Material Studio software. In addition, the specific surface areas of CoTAPc-PDA, CoTAPc-BDA and CoTAPc-TDA are 62, 81 and 137 m2 g−1, respectively. With increase in the frame size, the specific surface area of the corresponding material increases, which is bound to produce different electrochemical behaviors. Consequently, the initial capacities of the CoTAPc-PDA, CoTAPc-BDA and CoTAPc-TDA electrodes in lithium-ion batteries (LIBs) are 204, 251 and 382 mA h g−1, respectively. As the charge and discharge processes continue, the active points in the electrode material are continuously activated, leading to a continuous increase in charge and discharge capacities. After 300 cycles, the CoTAPc-PDA, CoTAPc-BDA and CoTAPc-TDA electrodes exhibit capacities of 519, 680 and 826 mA h g−1, respectively, and after 600 cycles, the capacities are maintained at 602, 701 and 865 mA h g−1, respectively, with a stable capacity retention rate at a current density of 100 mA g−1. The results show that the large-size frame structure materials have a larger specific surface area and more favorable lithium ion transmission channels, which produce greater active point utilization and smaller charge transmission impedance, thus showing larger charge and discharge capacity and superior rate capability. This study fully confirms that frame size is a key factor affecting the properties of organic frame electrodes, providing design ideas for the development of high-performance organic frame electrode materials.
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MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Luo lixia,Ye ying,Wang hong,Liu zhe,Li Jiqian
A cholesteric chiral artificial receptor L5 was synthesized, which recognized and cooperated with Ag + in metal ions, and a rapid method for detecting Ag + was established in food. It was found by fluorescence spectroscopy analysis that the L5 could recognize Ag + in DMSO solution; with the help of fluorescence and UV titration, job test and interference test to verify its recognition pattern, and founded that the L5 and guest Ag + were combined with 1:1 coordination ratio. Then, the recognition mechanism between L5 and guest Ag + was explored by measures of nuclear magnetic titration, infrared spectroscopy, electron microscopy and computer molecular simulation. It was speculated that the carbonyl oxygen atom near the amide of the MeO-PhCONH group and the carbonyl oxygen atom of the –COOCH 3 group cooperated with Ag + throµgh electrostatic gravitational interaction. This method was used to establish the detection of Ag + in food in which the detection limit of L5 for Ag + was derived as 0.13 µmol/L, and the silver ions in wolfberry, milk powder,wheat flour, tea leaf and soybean were accurately detected. This method can be used to quantify Ag + content in actual samples accurately and efficiently.
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Polymer Chemistry
·
2023
·Vol. 14
·期 14
·1665-1679
·
IF 4.6
Jiaming Liu,Xiaohong Liu,Xiaohua Cui,Jingjing Qin,Mengqin Wu,Lifu Fu,Min Shi,Dingsong Wang,Liyan Liang
Using biomass resources to prepare thermosets seems to have become a trend in the future of a sustainable society, and an active ester may be an excellent epoxy hardener for the electronic packaging field. In this work, we synthesized a resveratrol-derived epoxy (REP) and two resveratrol-derived active ester hardeners (triacetyl resveratrol (TAR), tri(m-toluoyl) resveratrol (TTR)), and then two resveratrol-derived bio-based epoxy thermosets (REP/TAR, REP/TTR) were prepared by the curing reaction of the epoxy and the hardener. The properties and structures of the thermosets were characterized and investigated. Results showed that the properties of REP/TAR in all aspects were better than those of REP/TTR; to be specific, the REP/TAR exhibited a higher gel fraction and better solvent resistance, indicating its better cross-linked network; the glass transition temperature of REP/TAR was higher and reached 177 °C (DMA) and the thermal stability of TEP/TAR was also better and the char yield at 600 °C was 46.5%. The main reason could be that the steric hindrance of acetyl groups in REP/TAR was smaller than that of m-toluoyl groups in REP/TTR. What's more, a novel analytical method was proposed for use in thermogravimetric analysis (TGA) to analyze the degradation process of thermosets, revealing a degradation process that was unique to the active ester cured epoxy thermosets. In all, the resveratrol-derived biobased epoxy thermosets could be a promising candidate for replacing fossil-derived thermosets and have potential application in the electronic packaging field, and the study on active ester hardeners might inspire the design and synthesis of subsequent active ester hardeners.
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ADVANCED MATERIALS
·
2023
·Vol. 35
·期 24
·2300526
·
IF 29.4
Zhuohua Dai,Guangfa Wang,Fangfang Xiao,Da Lei,Xincun Dou
Amorphous metal-based nanostructures have attracted great attention recently due to their facilitative electron transfer and abundant reactive sites, whereas it remains enigmatic as to whether amorphous copper-based nanoparticles (CuNPs) can be achieved. Here, for synthesizing amorphous CuNPs, glutathione is adopted as a ligand to inhibit the nucleation and crystallization process via its electrostatic repulsion. By subtly tailoring the solvent polarity, not only can amorphous glutathione-functionalized CuNPs (GSH-CuNPs) with phosphorescent performance be achieved after transferring the non-conjugation of GSH ligand to through-space conjugation, namely clusterization-triggered emission, but also the phosphorescence-off of GSH-CuNPs toward 2,4,6-trinitrotoluene (TNT) can be realized by the photoinduced electron-transfer process through the hydrogen bond channel, which is established between carboxyl and amino groups of GSH-CuNPs with the nitryl group of TNT. Benefitting from the intrinsic superiorities of the amorphous CuNPs, desired phosphorescence and detection performances of GSH-CuNPs toward airborne TNT microparticulates are undoubtedly realized, including high quantum yield (13.22%), excellent specificity in 33 potential interferents, instantaneous response, and ultralow detection limit (1.56 pg). The present GSH-CuNPs are expected to stretch amorphous metal-based nanostructures and deepen the insights into amorphous materials for optical detection.
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JOURNAL OF CHROMATOGRAPHY A
·
2023
·
IF 4.1
Zhen Wang,Wei Wang,Liquan Sun,Bo Tang,Fulai Zhang,Aiqin Luo
Herein, a chiral multishelled mesoporous carbon nanospheres (MCNs) with unique spiral multishelled hollow mesoporous chiral structure is synthesized; the MCNs can be used as stationary phases for high-resolution gas chromatography (GC) and have good separation capacity. The successful preparation of MCNs is verified by a variety of characterizations. In addition, the MCNs-coated capillary column shows excellent separation performance for n-alkanes, n-alcohols, aromatic compounds, and esters, and it has a faster analysis time than the HP-5 commercial capillary column. The chromatography separation performance for various isomers and racemates of the MCNs stationary phase was evaluated, and it showed good separation capability for amino acid derivatives. The MCNs-coated capillary column has been demonstrated to present good reproducibility and stability. In summary, all of the chromatography experiments in this work indicate that this new stationary phase of the MCNs has good application potential for GC capillary separation.
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MOLECULES
·
2023
·Vol. 28
·期 4
·1911
·
IF 4.6
Xiaocui Wu,Guishan Lin,Wengui Duan,Baoyu Li,Yucheng Cui,Bo Cen,Fuhou Lei
Twenty-two novel longifolene-derived diphenyl ether-carboxylic acid compounds7a–7vwere synthesized from renewable biomass resources longifolene, and their structures were confirmed by FT-IR,1H NMR,13C NMR, and HRMS. The preliminary evaluation of in vitro antifungal activity displayed that compound7bpresented inhibition rates of 85.9%, 82.7%, 82.7%, and 81.4% againstAlternaria solani, Cercospora arachidicola,Rhizoctonia solani,andPhysalospora piricola, respectively, and compound7lpossessed inhibition rates of 80.7%, 80.4%, and 80.3% againstR. solani,C. arachidicola,P. piricola, respectively, exhibiting excellent and broad-spectrum antifungal activities. Besides, compounds7fand7ashowed significant antifungal activities with inhibition rates of 81.2% and 80.7% againstA.solani, respectively. Meanwhile, a reasonable and effective 3D-QSAR mode (r2= 0.996,q2= 0.572) has been established by the CoMFA method. Furthermore, the drug-loading complexes7b/MgAl-LDHwere prepared and characterized. Their pH-responsive controlled-release behavior was investigated as well. As a result, complex7b/MgAl-LDH-2exhibited excellent controlled-releasing performance in the water/ethanol (10:1, v:v) and under a pH of 5.7.Keywords:longifolene;hydrotalcite;antifungal activity;3D-QSAR;controlled-releasing
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BIOCHEMICAL PHARMACOLOGY
·
2022
·
IF 6.1
Yi Li,Wenyan She,Tangxi Guo,Tianhe Huang,Yixin liu,Pan Liu,Xiaoran Xu,Xinyu Wang,Miao Wang,Chaochao Yu,Yi Liu,Yongchang Wei
Developing novel drugs for gastric cancer (GC) is greatly needed, and a reactive oxygen species (ROS)-modulating strategy has been demonstrated to be useful for cancer treatment. However, no organic arsenical-derived ROS-modulating drug has been developed in GC. Here, we constructed ACZ2 and investigated its efficacy and potential mechanism for GC in vitro and in vivo. Our data showed that ACZ2 could inhibit GC proliferation and cause G2/M phase arrest. Moreover, ACZ2 induced ROS accumulation by depleting glutathione (GSH) and TrxR1, triggering a subsequent ER stress response by activating the PERK/EIF2/ATF4/CHOP signalling pathways, which is a crucial step for ACZ2-mediated apoptosis and autophagy. Vitally, ROS scavenger (NAC) and ER stress inhibitor (4PBA) reversed ACZ2/ROS/ER stress-mediated apoptosis and autophagy. Our in vivo results clearly demonstrated that ACZ2 suppressed tumour growth in a GC xenograft model. Collectively, our data indicated that ACZ2 is a potential agent against GC.
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LUMINESCENCE
·
2023
·Vol. 38
·期 2
·159-165
·
IF 2.9
Linlin Lv,Weiwei Luo,Yixiao Zhou,Tiechun Li,Quanping Diao,Pinyi Ma,Daqian Song
Hydrazine (N 2 H 4 ) is a highly toxic and harmful chemical reagent. Fluorescent probes are simple and efficient tools for sensitive monitoring of N 2 H 4 enrichment in the environment, humans, animals, and plants. In this work, a ratiometric fluorescent probe (FP-1) containing coumarin was used for hydrazine detection. The proposed FP-1 probe had a linear detection range of 0–250 μM and a limit of detection (LOD) of 0.059 μM (1.89 ppb). A large red Stokes shift was observed in fluorescence and UV–vis absorption spectra due to the hydrolysis of ester bonds between FP-1 and hydrazine. The hydrazine detection mechanism of FP-1 was also investigated using density functional theory (DFT) calculations. Finally, FP-1 could sensitively and selectively monitor hydrazine in actual water samples and BEAS-2B cells. Therefore, it has great application potential in environmental monitoring and disease diagnosis.
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JOURNAL OF POLYMERS AND THE ENVIRONMENT
·
2023
·
IF 5.3
Song Jie,Zhang Rong,Han Jiaxuan,Dou Yufang,Yu Shuang,Ma Xiaoyan
To improve the performance of biodegradable materials and endow them with functionality, luteolin (Lc) was modified by esterification with acetyl chloride (Ac), iso butyryl chloride (Ic), benzoyl chloride (Bc) to improve its hydrophilicity and hydrophobicity, and Ac-L, Ic-L and Bc-L esters were obtained. The three esterified compounds were characterized and blended with PBS to prepare PBS/Ac-L, PBS/Ic-L and PBS/Bc-L composites. Studied the interface interaction mechanism, crystallization performance, thermodynamic performance, hydrophilic properties, and antibacterial performance between composite materials. The results showed that the majority of Ac-L, Ic-L, and Bc-L were dispersed in the PBS matrix, with a tighter two-phase interface and higher dispersibility. There were electrostatic adsorption, hydrogen bond and other interactions in the composite system, and the Intermolecular force became stronger and the compatibility increased. The introduction of Ac-L, Ic-L, and Bc-L did not change the crystal structure of PBS, but the crystallization rate and crystallinity of the composite material increased. The thermal decomposition temperature of composite materials increased, and the thermal stability and mechanical properties were further enhanced. With the increase of the amount of Ac-L, Ic-L, and Bc-L added, the antibacterial and hydrophobic properties gradually enhanced, making it suitable for use as a preservation and antibacterial material.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
·
IF 8.2
Jia Liu,Juan Yu,Chaoqun Xu,Bowen Li,Liang Liu,Chuanwei Lu,Yimin Fan
Due to the existence of water, it is still a challenge to conduct chemical modification on cellulose nanofiber (CNF) hydrogels with active double bonds. A simple one-pot and one-step method for constructing “living” CNF hydrogel with double bond was created at room temperature. The chemical vapor deposition (CVD) of methacryloyl chloride (MACl) was used to introduce physical-trapped, chemical-anchored and functional double bonds into TEMPO-oxidized cellulose nanofiber (TOCN) hydrogels. TOCN hydrogel could be fabricated within just 0.5 h, the minimum dosage of MACl could be reduced to 3.22 mg/g (MACl/TOCN hydrogel). Furthermore, the CVD methods showed high efficiency for mass production and recyclability. Moreover, the chemical “living” reactivity of the introduced double bonds were verified by the freezing and UV crosslinking, radical polymerization and thiol-ene click reaction. Compared with pure TOCN hydrogel, the obtained functionalized TOCN hydrogel exhibited remarkable improvements in mechanical properties, with enhancements of 12.34 times and 2.04 times, as well as an increase in hydrophobicity by 2.14 times and a fluorescence performance improvement of 2.93 times.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Jie Zhang,Yingying Li,Jingyu Hu,Yuanqiang Sun,Ran Yang,Zhaohui Li,Lingbo Qu
Phosgene is a very dangerous but important industrial intermediate and is a significant threat to public health. There is, therefore, an urgent need to develop a rapid, visual, and on-site detection method for phosgene. Sensitive and selective phosgene responsive carbon dots (CDs) were synthesized by employing 2-nitro-4-aminodiphenylamine as precursors. The amine group of the CDs can interact selectively with phosgene to effect acylation reactions, which cause color changes from yellow to amaranth and remarkable changes in fluorescence from bright yellow to orange-red due to modification of the CDs’ intramolecular charge transfer (ICT) process. The CDs exhibited fast response (<2 s) for detection of phosgene with an ultralow detection limit (0.63 nM). Furthermore, a portable CD/polystyrene droplet system was developed for rapid and on-site visualization of phosgene. Specifically, the droplet system not only can realize rapid on-spot visual inspection of gaseous phosgene in the liquid phase with the naked eye, but also could make long-term visualization in the solid phase via a polystyrene membrane after solvent volatilization. This study has expanded the scope for application of CDs in sensing field, and provides a new and effective strategy for fabrication excellent platform for real-time detection of phosgene leakage in industrial and public safety applications.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2022
·
IF 9.221
Yingying Li,Jie Zhang,Zengqiang Liang,Ran Yang,Lingbo Qu,Zhaohui Li,Yuanqiang Sun
It is of great significance for real-time monitoring of phosgene to protect public safety. In this paper, a new rhodamine derivate with highly rapid, special and sensitive response towards phosgene was synthesized and used as a phosgene probe based on its spirolactam ring-opening property and nucleophilic reaction with phosgene. To realize in situ visualization of phosgene, a fluorescent detection pen with gas-liquid reaction model was proposed for the first time using the mixture of the probe and polystyrene as ink. The detection film could be formed in situ by simply writing on desired surface and respond toward phosgene gas within 30 s with an ultra-low detection limit (2 ppm) with the naked eye. Such a fluorescence pen detection mode supplied a new strategy for the fabrication of an excellent platform for real-time detection of phosgene and other gas analytes.
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