MACROMOLECULAR CHEMISTRY AND PHYSICS
·
2021
·Vol. 222
·期 23
·2100284
·
IF 2.527
Da Zhang,Jinxin Zheng,Pengfei Zhang,Ronghui Zhao,Zhuo Chen,Meng Wang,Kuilin Deng
In the synthesis of traditional AIE-active polymers with conjugate or multi-benzene system, the troublesome process is still faced such as consuming time, high temperature, catalysis, no water or vacuum, and so on. In this study, the polydihydropyrimidone derivatives (PDPMDs) with AIE properties are facilely synthesized by the introduction of 4-dihydropyrimidone rings onto non-AIE-active intermediate polyureas (PUs) in Biginelli reaction. It is found that the unsymmetrical L- lysine ethyl diisocyanate and butylenediamine played a very important role in the smooth preparation and fluorescence enhancement of PDPMDs. Compared with the intermediate PUs, the fluorescence of PDPMDs is significantly enhanced (35-fold increase), which is mainly due to the intramolecular aggregation of dihydropyrimidone rings on PUs chains. At the same time, with the increase of the content of dihydropyrimidone rings, the fluorescence intensity of PDPMDs also increases, and the emission wavelength shows an obvious red shift. The fluorescence of PDPMDs also showed obvious dependence on excitation wavelength, which further reveals the clusterization-triggering emission (CTE) mechanism. In summary, the strategy of endowing AIE properties to non-AIE active polymer by introducing heterocycles into the backbone through multi-component reaction provides useful guidance for AIE functionalization of other non-AIE materials.
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高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2018
·
IF 3.235
Xiaoming Chen,Mingdi Yang,Qishu Qu,Qingchun Zhao,Wensheng Zou
The synthesis and electrochromic properties of a novel regiosymmetric polymer based on 3,4-ethylenedioxythiophene, poly(2,3-bis(bromomethyl)-2,3-dihydrothieno[3,4-b][1,4]dioxine) (PEDOT(MeBr) 2 ) were highlighted. The monomer was electrochemically polymerized via repetitive cycling between 0 and 1.8 V in lithium perchlorate (LiClO 4 )–acetonitrile (ACN) electrolytic medium. The corresponding polymer was characterized by FTIR spectra, scanning electron microscopy, cyclic voltammetry , UV–Vis-NIR spectroscopy and colorimetry . It features a reversible redox process and demonstrates a stable blue-to-transmissive electrochromic behavior with very low driving potentials (−0.1 and 0.65 V). Additionally the polymer film exhibits enhanced optical contrast (60% at 669 nm) and improved coloration efficiency (183.1 cm 2 /C at 100% full contrast during bleaching process) which are higher than those of PEDOT, a relatively longer response time compared with PEDOT and reasonable redox stability.
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高影响因子
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2024
·
IF 5.7
Bo Luo,Yuerui Wu,Xinran Ren,Huimin Li,Xuanru Li,Gege Wang,Mengjia Wang,Luqi Dong,Mengxing Liu,Wei Zhou,Lailiang Qu
In the search for novel succinate dehydrogenase inhibitor (SDHI) fungicides to control Rhizoctonia solani, thirty-five novel pyrazole-4-carboxamides bearing either an oxime ether or an oxime ester group were designed and prepared based on the strategy of molecular hybridization, and their antifungal activities against five plant pathogenic fungi were also investigated. The results indicated that the majority of the compounds containing oxime ether demonstrated outstanding in vitro antifungal activity against R. solani, and some compounds also displayed pronounced antifungal activities against Sclerotinia sclerotiorum and Botrytis cinerea. Particularly, compound 5e exhibited the most promising antifungal activity against R. solani with an EC50 value of 0.039 μg/mL, which was about 20-fold better than that of boscalid (EC50 = 0.799 μg/mL) and 4-fold more potent than fluxapyroxad (EC50 = 0.131 μg/mL). Moreover, the results of the detached leaf assay showed that compound 5e could suppress the growth of R. solani in rice leaves with significant protective efficacies (86.8%) at 100 μg/mL, superior to boscalid (68.1%) and fluxapyroxad (80.6%), indicating promising application prospects. In addition, the succinate dehydrogenase (SDH) enzymatic inhibition assay revealed that compound 5e generated remarkable SDH inhibition (IC50 = 2.04 μM), which was obviously more potent than those of boscalid (IC50 = 7.92 μM) and fluxapyroxad (IC50 = 6.15 μM). Furthermore, SEM analysis showed that compound 5e caused a remarkable disruption to the characteristic structure and morphology of R. solani hyphae, resulting in significant damage. The molecular docking analysis demonstrated that compound 5e could fit into the identical binding pocket of SDH through hydrogen bond interactions as well as fluxapyroxad, indicating that they had a similar antifungal mechanism. The density functional theory and electrostatic potential calculations provided useful information regarding electron distribution and electron transfer, which contributed to understanding the structural features and antifungal mechanism of the lead compound. These findings suggested that compound 5e could be a promising candidate for SDHI fungicides to control R. solani, warranting further investigation.
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PubMed
高影响因子
Journal of Nano Research
·
2021
·
IF 2.929
Bi Quan Su,Yinxia feng,Liang Xian,Li Sheng,Qi Qi Li
Photochemistry to prepare platinum nanoparticles (Pt NPs) is an essential way to control Pt NPs catalyst size distribution. This article reports a series of morphologically controlled syntheses of Pt NPs loaded on modified carbon nanotube (Pt-CNTs). In the synthesis, Polyethylene glycol (PEG) participates in reactions both as a reducing agent and a stabilizer. Visible light irradiation was adopted as a kinetic controlling approach. Typical 4-nitrophenol (4-NP) reduction was adopted to probe the catalytic performances. Characterizations prove that visible light irradiation is an effective way to control the reaction process. In the optimized reaction conditions, i.e., when the ratio PEG:H2O is 1:9, and the pH is 10, the as-prepared Pt NPs are consequently in a very narrow sized distribution with an average diameter of 1.29 nm. The Pt-CNTs present a high reaction rate constant of 0.624 min-1 in the catalytic reduction of 4-NP. All the research results are beneficial for exploring more green chemistry and facile photochemical approaches in the controlled preparation of Pt nanocatalysts.
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高影响因子
Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Yuwei Xue,Lihua Liu,Ting Zhang,Ziqi Zhu,Mingjun Xu,Qian Zhang,Junming Hong
There has been growing attention in the combination of metal oxide nanoparticles with metal-organic frameworks (MOFs) for the synergistically intensified catalytic activity . Herein, functional Fe-MOF@Mn 2 O 3 composites were synthesized to activate peroxymonosulfate (PMS) for 4-Cholophenol (4-CP) degradation via a hydrothermal and calcination method. Under the reaction parameters of 2 mM PMS, 0.2 g/L catalyst dosage, and pH 7.0, 91.4% of 4-CP (10 mg/L) could effectively be degraded within 60 min (2.2-fold increase in reaction rate constant compared with pure Mn 2 O 3 ). The excellent degradation performance of Fe-MOF@Mn 2 O 3 /PMS system was attributed to the surface hydroxyl and synergistic effect between iron and manganese. Quenching reaction and EPR analysis revealed both sulfate (•SO 4 - ) and hydroxyl radicals (•OH) were responsible for 4-CP degradation. The Fe-MOF@Mn 2 O 3 composite exhibited intensive catalytic capability as well as electron transfer efficiency according to the electrochemical measurements. Meanwhile, the possible degradation pathways were proposed by analyzing intermediates via LC-MS detection. The results indicates that the Fe-MOF@Mn 2 O 3 /PMS system is effective and adaptable for the treatment of 4-CP in different water conditions.
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高影响因子
ChemistrySelect
·
2024
·Vol. 9
·期 36
·e202401875
·
IF 1.9
Haonan Li,Chenping Gao,Qingjie Liu,Yanchun Guo,Yufen Zhao
Graphical We report here a new I 2 /H 2 O 2 co-catalyzed oxidative [4+1] cyclization of benzaldehyde with 2-(aminomethyl)pyridine or o -phenylenediamine/2-aminothiophenol to provide various substituted imidazo[1,5- a ]pyridines and benzimidazoles/thiazole via C(acyl)−N bond construction. Some of heterocyclic products exhibit blue luminescence properties, as well as large Stokes shifts, eminent fluorescence quantum yields (64 %) and long fluorescence lifetimes. An efficient I 2 (10 mmol %)/H 2 O 2 mediated oxidative formal [4+1] cyclization of 2-pyridinemethylamine or o -phenylenediamine (2-aminobenzenethiol) with benzaldehyde via C−N bond formation has been developed. This strategy provides a straightforward approach to imidazo[1,5- a ]pyridines, iodo-substituted imidazo[1,5- a ]pyridines and benzimidazole (benzothiazole) derivatives in yields ranging from 60 % to 98 %, respectively. Several heterocyclic products exhibit promising blue luminous performance with satisfactory fluorescence quantum yields of up to 64 %, large Stokes shifts, and a longer lifetime (7.35 ns). The band gap energies obtained from DFT are also consistent with the absorption spectra.
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高影响因子
ChemistrySelect
·
2024
·Vol. 9
·期 47
·e202404091
·
IF 1.9
Rui Wang,Jiali Yuan,Huan Zhang,Xiang Liu,Jiani He,Lihua Zhu
Graphical Th Pd/NC catalysts with different Pd loadings were synthesized via sodium borohydride liquid-phase reduction method. Among of the catalysts, 2.52%Pd/NC catalyst exhibits the best performance and high stability in the 4-nitrophenol hydrogenation reaction with TOF = 321.8 h −1 and 100% selectivity at high conversion of 4-nitrophenol. A series of the Pd/NC samples with various Pd loadings (0.11%, 0.48%, and 2.52%) are prepared via sodium borohydride (NaBH 4 ) reduction method and carbon doping with nitrogen (NC) is acquired by the pyrolysis of ZIF-8. The samples are characterized by XRD, BET, SEM, TEM, HRTEM, STEM-EDX elemental maps and line-scanning, XPS, TG, and so forth. It confirms that the Pd nanoparticles (NPs) are successfully coated on the NC. The catalytic behaviors of the samples are evaluated by the hydrogenation of 4-nitrophenol (4-NP), the 2.52%Pd/NC catalyst shows the best catalytic property among as-obtained catalysts maybe due to the much more Pd(0) species. The 2.52%Pd/NC catalyst exhibits 100% selectivity to 4-aminophenol (4-AP) at high conversion of 4-nitrophenol and 321.8 h −1 turnover frequency (TOF) under mild reaction conditions (3.0 MPa H 2 , 40 °C, 1 h). Moreover, the catalysts show an excellent stability.
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高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2019
·
IF 4.978
Xian-Fei Huang,Guang-Ping Yuan,Guan Huang,Su-Juan Wei
Aiming at the most enhancing the catalytic performance of simple and cheap cobalt(II) 5,10,15,20-tetrakis(4-pyridyl)porphyrin (Co TPyP), guided by the nowadays-advanced various technologies, Co TPyP was anchored onto nanoporous bar with thiol-functionalized silica (npb-SiO 2 -SH). The resulting npb-SiO 2 -S-Co TPyP catalyst was characterized using various techniques, determining its structure. The total surface area ratios (TSAR) of the immobilized cobalt porphyrin to the npb-SiO 2 -SH, and the catalytic cyclohexane oxidation reaction conditions were at the same time optimized via Response Surface Methodology (RSM). Compared with those obtained from traditional optimizing method (TOM), on average, RSM could enhance as high as more than 60% catalyst turnover frequency (TOF) and yields of cyclohexanone and cyclohexanol (KA oil). The anchored 0.05 mg Co TPyP could catalyze the oxidation of 200 mL of cyclohexane, under not using any solvents and additives, offering 2.5 × 10 6 1/h of TOF, and 19% of yields. The npb-SiO 2 -S (20%-0.0438)-Co TPyP catalyst showed better reusability, excellent catalytic
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高影响因子
CARBON
·
2018
·
IF 7.082
Yuanyuan Zhang,Peng Yan,Qijin Wan,Nianjun Yang
Metal-organic frameworks (MOFs) are attractive materials for electrochemical applications because of their large surface areas and rich pore structures . However, their poor electrical conductivity hinders these applications. In this contribution, the decoration of chromium terephthalate MOFs (MIL-101(Cr) crystals) with reduced graphene oxide (rGO) is proposed to improve the electrical conductivity of MIL-101(Cr) crystals. These nanocomposites (MIL-101(Cr)@rGO) were prepared using a simple chemical reduction method. Their morphology, interfacial properties , and electrochemical applications were investigated using electron microscopy , electrochemical, and related techniques. With an introduction of rGO into MIL-101(Cr) crystals, the conductivity of MIL-101(Cr)@rGO nanocomposites was much improved. As a case study of electrochemical applications of MIL-101(Cr)@rGO nanocomposites, the MIL-101(Cr)@rGO nanocomposite coated electrodes were employed for the voltammetric study of 4-nonylphenol. An irreversible, adsorption-controlled, one electron and one proton involved oxidation process was observed. By use of the recorded anodic peak current as the physical parameter, the sensitive and reproducible monitoring of 4-nonylphenol was realized in the range of 0.1–12.5 μM with a detection limit of 33 nM. The MIL-101(Cr)@rGO nanocomposites are thus useful electrode materials . The proposed strategy provides a simple and efficient approach to expand easily the applications of MOFs into various electrochemical fields.
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高影响因子
JOURNAL OF ORGANIC CHEMISTRY
·
2022
·
IF 4.198
Bin Sun,Xiaohui Zhuang,Jieli Yin,Kesheng Zhang,Haiyun Zhao,Can Jin
The photoredox-catalyzed radical difluoroalkylation/cyclization/hydroxylation cascade reaction of various 2-bromo-2,2-difluoro-N-arylacetamides containing unactivated alkene moieties has been developed, providing green and efficient access to various 4-hydroxyalkyl-3,3-difluoro-γ-lactams. Control experiments confirmed a radical process, and inexpensive air acted as the sole hydroxy resource. In addition, the highlights of this protocol include good tolerance for a variety functional groups, lower photocatalyst loading, and ease of operation.
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高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Yu-Xuan Dai,Wen-Li Xin,Lian-Hua Xu,Ji Li,Yi-Xuan Li,Junji Li,Serge Cosnier,Xue-Ji Zhang,Robert S. Marks,Dan Shan
Rational design highly active transition metal or transition metal oxides/nanocarbon hybrids is one of the feasible way to deliver a cooperative oxygen reduction (ORR) with a synergistic effect of the hybrid interface. Herein, based on benzimidazole-5-carboxylate (BIMC), CoO/Co-N-C nanocomposites are fabricated via 2-methylimidazole (2-MeIm)-tuned “4-Self” strategy, namely, self-templating, self-adapting, self-assembly and self-catalysis. As a base competitive ligand with N and C sources, 2-MeIm modulates the dispersion of BIMC in methanol to generate collodial-like BIMC tiny particles, the coordination ability of BIMC to Co(II), the composition and morphology of the self-assembled precursor (Co-BM), and as well as the conductivity of the resultant electrocatalyst. Impressing, carbonization of Co-BM at 800 °C under N 2 atmosphere endows the pyrolysis product (Co-BM-800) with the well-dispersed Co/CoO riveted on nitrogen-doped carbon, as well as the enhanced ORR performance in terms of positive onset-potential (0.890 V vs. RHE), large diffusion limiting current density (5.21 mA cm −2 ), and high stability.
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高影响因子
ChemElectroChem
·
2020
·Vol. 7
·期 17
·3656-3662
·
IF 4.154
Shufeng Song,Xinjie Tan,Yanfang Zhai,Guanming Yang,Jianyao Yao,Shuai Li,Ning Hu,Xueli Qi,Ru Li,Wandong Ma,Zhaoyin Wen,Li Lu
Graphical Must gel polymer electrolyte membranes be porous? Ultrathin and compacted gel polymer electrolyte with robust chemical interaction between SiO 2 nanoparticles and poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) chains enables a wide electrochemical stability window and excellent cycling stability. Batteries with lithium metal as anodes and gel polymer membranes as electrolytes are promising, because of their high energy densities and improved safety. To achieve metal battery energy densities that are comparable to liquid-electrolyte batteries, ultrathin and lightweight gel electrolytes with wide electrochemical stability windows are desired. However, it is challenging to make gel polymer electrolyte membranes with comparable thicknesses to commercial polymer electrolyte separators (<20 μm), because of the porous configuration and increased risk of short-circuiting cells. Here, we report on a 10 μm-thick compacted gel polymer electrolyte (TCGPE), demonstrated to have a robust chemical interaction between SiO 2 nanoparticles and poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) chains that are activated via an in situ sol-gel reaction. The developed TCGPE exhibits an extremely wide electrochemical stability window of 5.5 V vs. Li/Li + and prevents the batteries from short-circuiting even at a high current density of 1.0 mA cm −2 . Moreover, Li/TCGPE/LiNi 0.5 Co 0.2 Mn 0.3 O 2 shows an excellent capacity retention of 99.8 % after 180 cycles at 1 C rate.
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高影响因子
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