RSC Advances
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2023
·Vol. 13
·期 18
·11938-11947
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IF 3.9
Yu Liang,Wanrui Gui,Zhihong Yang,Kang Cheng,Xin Zhou,Can Yang,Jianmei Xu,Wei Zhou
Designing organic–inorganic hybrid semiconductors is an effective strategy for improving the performance of the photocatalyst under visible light irradiation. In this experiment, we firstly introduced Cu into perylenediimide supramolecules (PDIsm) to prepare the novel Cu-dopped PDIsm (CuPDIsm) with one-dimensional structure and then incorporated CuPDIsm with TiO2 to improve the photocatalytic performance. The introduction of Cu in PDIsm increases both the visible light adsorption and specific surface areas. Cu2+ coordination link between adjacent perylenediimide (PDI) moleculars and H-type π–π stacking of the aromatic core greatly accelerate the electron transfer in CuPDIsm system. Moreover, the photo-induced electrons generated by CuPDIsm migrate to TiO2 nanoparticles through hydrogen bond and electronic coupling at the TiO2/CuPDIsm heterojunction, which further accelerates the electron transfer and the separation efficiency of the charge carriers. So, the TiO2/CuPDIsm composites exhibit excellent photodegradation activity under visible light irradiation, reaching the maximum values of 89.87 and 97.26% toward tetracycline and methylene blue, respectively. This study provides new prospects for the development of metal-dopping organic systems and the construction of inorganic–organic heterojunctions, which can effectively enhance the electron transfer and improve the photocatalytic performance.
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TALANTA
·
2023
·
IF 6.1
Zhilan Zhou,Ya Wang,Zhengtao Shao,Guixi Zhang,Hang Jiang,Yiyuan Tang,Zening Huang,Yingdi Zhu,Juan Li
Drug resistance is a worldwide health care crisis which impedes disease treatment and increases financial burden, especially for its multifactorial nature and high complexity. Herein, we developed a multiparametric approach to visualize and detect drug resistance in living cancer cells, through the combination of DNA-templated covalent protein labeling strategy and fluorescent resonance energy transfer technique. Gefitinib resistance in non-small cell lung cancer caused by mesenchymal-epidermal transition factor (Met) overexpression and hyperactivation was investigated as a proof-of-concept. Unlike the traditional single-factor investigation, the proposed approach evaluated the contribution of three important parameters towards the resistance, including the changes of Met expression level, the homodimerization of Met with itself and the heterodimerization of Met with epidermal growth factor receptor (EGFR). A multiple regression model based on these three parameters was tentatively established for evaluation of the resistance level of laboratory-developed resistant cells and evaluation of the resistance level of patient-derived cells. Such an approach facilitates a quick identification of a drug resistance, to evaluate not only the resistance level but also the resistance mechanism.
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Catalysts
·
2023
·Vol. 13
·期 5
·799
·
IF 3.9
Tao Wang,Jie Li,Hanwen Yan,Guoliang Zhang,Shifeng Li
Methacrolein (MAL) is an important intermediate extensively used in the manufacture of methyl methacrylate and other materials (polymers and resins). In this study, a series of secondary amines/acids were explored as catalysts for the condensation of formaldehyde and propionaldehyde to prepare MAL. It was found that the structure of the amines and acids directly affected the yield of MAL. The effect of the catalyst was closely related to the nucleophilicity of the amines as well as the steric hindrance effect, while acids also played a role as co-catalysts. Dibutylamine acetate was selected as the catalyst after investigation. The catalytic performance of the system was systematically studied by a series of single-factor experiments, including stirring rate, temperature, reaction time, acid/amine ratio, and the solvent, and the optimized reaction conditions were obtained. In the optimum condition, the yield of MAL was up to 97.3%. Kinetic experiments were performed for the condensation of formaldehyde and propionaldehyde to MAL, and the activation energies, reaction orders, and rate-limiting step of the reaction were determined. The results indicate that the decomposition of the Mannich base is a rate-limiting step.Keywords:methacrolein;aldol condensation;Mannich reaction;kinetics
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ANALYTICA CHIMICA ACTA
·
2023
·
IF 6.2
Meng Cheng,Caiwei Tan,Bo Xiang,Weihong Lin,Bolin Cheng,Xuechun Peng,Yihao Yang,Yongping Lin
Visualized gene detection based on the CRISPR‐Cas12/CRISPR‐Cas13 technology and lateral flow assay device (CRISPR‐LFA) has shown great potential in point‐of‐care testing sector. Current CRISPR‐LFA methodology mainly utilizes conventional immuno-based LFA test strips, which could visualize whether the reporter probe is trans -cleaved by Cas protein, indicating the target positive detection. However, conventional CRISPR‐LFA usually produces false-positive results in target negative assay. Herein, a nucleic acid C hain H ybridization‐based L ateral F low A ssay platform, named CHLFA, has been developed to achieve the CRISPR‐CHLFA concept. Different from the conventional CRISPR‐LFA, the proposed CRISPR‐CHLFA system was established based on the nucleic acid hybridization between the GNP‐probe embedded in test strips and ssDNA (or ssRNA) reporter from CRISPR (LbaCas12a or LbuCas13a) reaction, which eliminated the requirement of immunoreaction in conventional immuno-based LFA. The assay realized the detection of 1–10 copy of target gene per reaction within 50 min. The CRISPR-CHLFA system achieved highly accurate visual detection of target negative samples, thus overcoming the false-positive problem that often produced in assays using conventional CRISPR‐LFA. The CRISPR‐CHLFA platform was further adopted for the visual detection of marker gene from SASR‐CoV-2 Omicron variant and Mycobacterium tuberculosis (MTB), respectively, and 100% accuracy for the analysis of clinical specimens (45 SASR‐CoV-2 specimens and 20 MTB specimens) was obtained. The proposed CRISPR-CHLFA system could provide an alternative platform for the development of POCT biosensors and can be widely adopted in accurate and visualized gene detection.
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INORGANIC CHEMISTRY COMMUNICATIONS
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2023
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IF 3.8
Ziyang Lu,Bing Li,Xiaodie Zhu,Yangrui Xu,Jutao Zhang,Guosheng Zhou,Binghui Wei,Xinlin Liu,Jinyu Chu,Chundu Wu
Recyclable and stable imprinting modified PDI/ZnFe 2 O 4 (IM-PDI/ZFO) was assembled by mutual magnetic attraction. Interestingly, the obtained IM-PDI/ZFO exhibited granular ZnFe 2 O 4 (ZFO) attached to the aggregated PDI. The mutual magnetic attraction of ZFO leaded to the aggregation of PDI, which effectively improved the ability of IM-PDI/ZFO to enrich pollutants and further enhanced the photodegradation activity. Meanwhile, due to the appropriate energy band position, PDI and ZFO formed an S-scheme heterojunction, eliminating useless photogenerated charge carriers and enhancing the photodegradation ability of IM-PDI/ZFO. Most importantly, because of the introduction of imprinting modification technology, tetracycline (TC) was added during the synthesis process. The IM-PDI/ZFO obtained imprinted cavities consistent with the three-dimensional structure of TC, which was not only conducive to improve the photocatalytic activity under visible light, but also endowed IM-PDI/ZFO with high selectivity, the selectivity coefficient reached 2.31. This work presents an innovative viewpoint for the synthesis of magnetic imprinted S-scheme heterojunction photocatalysts.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Jing Chen,Jiakun Yang,Qin Wu,Daxin Shi,Kangcheng Chen,Yaoyuan Zhang,Xiaoyan Zheng,Hansheng Li
The cycloaddition reaction of CO 2 with epoxides is challenging, thereby requiring the development of environmentally friendly catalysts. Herein, a strategy was developed to construct a multifunctional heterogeneous magnetic catalyst (MPNPs-[ImR 2 NH 2 ][ZnBr 3 ]) of aminoethyl imidazole metal halide ionic liquids coated on nano-sized CoFe 2 O 4 @polystyrene for CO 2 cycloaddition. The created catalytic system displayed the intramolecular synergy of ternary active sites (Zn 2+ , Br − , and –NH 2 ), as well as coupling of catalysis and magnetic separation. In the absence of co-catalyst and solvent, MPNPs-[ImR 2 NH 2 ][ZnBr 3 ] exhibited excellent catalytic performance for CO 2 cycloaddition (99.92% yield and 100% selectivity) at 120 ℃ with 0.16 mol% catalyst dosage in 2.5 h. By appropriately increasing the reaction duration and catalyst dosage, 98.83% conversion and 99.26% selectivity were achieved even at mild conditions of 60 °C and 0.1 MPa. After 10 cycles of reuse, the recycled MPNPs-[ImR 2 NH 2 ][ZnBr 3 ] demonstrated the same high-efficiency activity as the fresh catalyst, as well as excellent stability and magnetic separation. Based on the density functional theory (DFT) calculations, the intramolecular synergy of ternary active sites and the catalytic mechanism of bimolecular activation based on the multifunctional structure were proposed. This excellent catalyst was attributed to the intramolecular synergy of ternary active sites, large loading of active centers, lower internal diffusion resistance, the inert protective effect of polystyrene layer and the easily magnetic separation of CoFe 2 O 4 , highlighting a new direction for green catalytic chemistry.
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RSC Advances
·
2023
·Vol. 13
·期 14
·9347-9352
·
IF 3.9
Yu-Fen Bao,Yi-Jie Wang,Yu-Chen Wang,Ding-Hua Liu
In the synthesis of dimethyl carbonate (DMC) by transesterification, CH3ONa has been commonly applied as a homogeneous catalyst due to its high catalytic activity, but its stability is unsatisfactory. Here, by studying the influence of ionic liquid base strength on transesterification, we prepared an organic base catalyst, potassium imidazole (KIm), with high catalytic activity and stability, which solved the problem of catalyst deactivation in transesterification. The results showed that when KIm was used in the synthesis of DMC from propylene carbonate (PC) and methanol (MeOH), the chemical equilibrium could be reached within 3 minutes and the yield of DMC reached 73.03%, indicating that KIm performed better in transesterification than the majority of previously reported catalysts. In addition, the activity of the catalyst had hardly decreased after ten cycles of reaction, which can well meet the requirements of industrial production.
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JOURNAL OF MOLECULAR LIQUIDS
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2023
·
IF 6
Liwei Cheng,Zhi Li,Jinlong Cui,Ran Zhu,Jia Li,Huibo Qin,Bei Liu,Guangjin Chen,Fulong Ning
In recent years, kinetic hydrate inhibitors (KHIs), as an important hydrate control method, have received extensive attention in the oil and gas industry. During the usage of KHIs, it is often necessary to add KHI synergists to maximize their hydrate inhibition performance. Therefore, the development of synergistic reagents with high-efficiency to improve inhibition performance of the KHIs is of great significance for the prevention and treatment of hydrates. In this work, we screened a series of imidazole reagents as KHIs synergists through experiments, and studied the synergistic mechanism between imidazole reagents and KHIs by molecular simulation. Our results demonstrate that the addition of low concentrations of imidazole reagents alone has no obvious inhibitory effect on methane hydrates, but show obvious synergistic hydrate inhibition effect with KHIs. Among the tested imidazole reagents, 2-propylimidazole shows the best synergistic effect with KHIs. The synergistic effect between 2-propylimidazole and KHIs is mainly reflected in two aspects. On the one hand, the adsorption of 2-propylimidazole molecules on the hydrate surface hinders the formation of hydrate. On the other hand, 2-propylimidazole molecules can promote the formation of methane bubbles and reduce the driving force for the formation of methane hydrates. Our research further expands the application of imidazole reagents in the prevention and control of hydrates, which is beneficial to enhance the commercial application of KHIs.
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JOURNAL OF POLYMER SCIENCE
·
2022
·Vol. 61
·期 6
·491-502
·
IF 3.046
Lidong Cao,Xingzhong Fang,Guofei Chen
High imidization temperature of polyimides (PIs) brings great restriction to the applications in electronic industry. In this study, N,N ′-carbonyldiimidazole (CDI), a novel low-temperature imidization accelerator with the unique dual function of catalyst and dehydrating agent, was researched to solve this problem. PIs synthesized from 4,4′-(hexafluoroisopropylidene)diphthalic anhydride (6FDA) and 4,4′-oxydianiline were researched as the main object on method A and method B, two preparation methods of PIs, by introduction of CDI, which was found that the PIs prepared by method A achieved complete imidization and basically had no residual CDI and N,N -Dimethylacetamide at 180 °C under vacuum, while the completely imidized PIs prepared by method B were also obtained at 40 °C. Even prepared at low temperature, the PI films with adding CDI both showed satisfactory thermal and mechanical properties, especially in reducing coefficient of thermal expansion. In addition, the universality of the reaction between CDI and poly(amic acid) were also verified by other soluble PI systems. All these results prove the superior performance of CDI in lowering imidization temperature, showing great potentials in low-temperature cured PIs. Graphical
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JOURNAL OF MOLECULAR LIQUIDS
·
2023
·
IF 6
Lihua Zhou,Xiangbin Fan,Yang He,Shaohua Gou,Qiankun Bi,Junwen Chen,Lei Chen,Jun wang,Hua Guo,Yuanpeng Wu,Hairong Yue,Xingfu Li
The long-term effect of protecting water-sensitive reservoirs and enhancing permeability of water invasion reservoir is still an urgent practical problem to be solved. Here, an imidazolium Gemini ionic liquid (IL), PEG-DC 8 Im, with octyl as tail chain and polyoxyethylene chain as bridging group, was synthesized to inhibit the hydration, swelling and dispersion of clay minerals. The PEG-DC 8 Im could exert excellent anti-swelling ability (93.82 %) and outstanding washable capacity (cumulative decrease of anti-swelling rate after being washed five times: 1.32 %) at the concentration of 60 mmol/L. The inhibition effect of 20 mmol/L PEG-DC 8 Im was significantly better than that of 250 mmol/L KCl at 90 °C. And the PEG-DC 8 Im could intercalate into the interlayer space of MMT through cation exchange to play an inhibition effect, where zeta potential of MMT particles was reduced and then the dispersion ability of MMT was weakened. Subsequently, the anionic polymer poly(AM/AA) was found to cooperate with PEG-DC 8 Im to improve the inhibition effect for MMT swelling and dispersion, in which poly(AM/AA) was not intercalated into the interlayer of MMT, and only adsorbed on the surface of the particles to encapsulate the MMT particles. Simultaneously, the apparent viscosity and thixotropy of the composite solution were enhanced. Besides, after the treatment of PEG-DC 8 Im, the displacement pressure decreased and the permeability of sandstone cores increased due to the inhibition of clay mineral hydration, revealing the enhancement of injectivity. Finally, the pore connectivity of the core increased and the water wettability was weakened. The treatment of PEG-DC 8 Im was conducive to the discharge of invasive water in reservoir and the improvement of the reservoir permeability. Overall, PEG-DC 8 Im has a good application prospect as permeability-enhancing clay stabilizers.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2023
·
IF 5.2
Feng Wang,Wei Hu,Sheli Zhang,Chunyan Zhu,Yunchang Fan,Qiang Wang
In the present work, a two-phase system composed of a hydrophobic ionic liquid (IL) containing copper ions (Cu(II)) and water containing organic linkers was constructed and the Cu-based metal-organic framework (Cu-MOF) formed at the IL-water interfaces at room temperature. The IL 1,3-bis(carboxymethyl)imidazolium chloride ([BCMIM]Cl) was also introduced in the MOF structures via using it as co-linker. The adsorption capacity of the synthesized Cu-MOF and [BCMIM]Cl modified Cu-MOFs was evaluated using the organic dye Congo red (CR) as target compound. Experimental results suggested that the incorporation of [BCMIM]Cl in the Cu-MOF remarkably improved the CR adsorption capacity due to the strong π-π and electrostatic interactions between the cation of [BCMIM]Cl and CR. The adsorption behavior of CR on [BCMIM]Cl modified Cu-MOF fitted well with pseudo-second-order kinetics and Freundlich isotherm model. Thermodynamic analysis suggested the adsorption of CR on [BCMIM]Cl modified Cu-MOF was a physical adsorption process . Finally, compared with reported adsorbents, the [BCMIM]Cl modified Cu-MOF exhibited higher CR adsorption capacity, indicating that it was a promising adsorbent for the removal of organic dyes from water.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Wenting Wu,Zongqi Zhang,Lipeng Sun,Ruiping Wei,Lijing Gao,Xiaomei Pan,Jin Zhang,Jin Yu,Guomin Xiao
Well-arranged photosensitive units and catalytic sites in closeness are critical for enhancing charge separation effectiveness and promoting photocatalysis. Here, a heterogeneous interface is constructed, which binds a deprotonated carboxyl group on perylene diimide (PDI) photosensitizer to unsaturated metal sites generated by etching of different Prussian blue analogues (PBAs). The atomically-dispersed metal sites and anchored photosensitive units greatly accelerate charge transfer. Typically, the S-scheme heterojunction built by etched NiCo PBA and PDI (NCSP) possesses bond of O-Ni. Density functional theory (DFT) and in-situ technology reveals the electron density of the Ni active site is optimized. Consequently, activation barrier of CO 2 on the Ni site was reduced, thus improving the CO generation (60.0 μmol g −1 ) up to about 9 times than NiCo PBA. This work reveals key insights into the precise modulation of active moiety for efficient photocatalytic CO 2 conversion.
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