DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 46
·17201-17212
·
IF 4
Qiu Lv,Qing Lin Guan,Jin Long Li,Jin Xiao Li,Jing Jin,Feng Ying Bai,Yong Heng Xing
Triazole polycarboxylic acid ligands are widely employed in the construction of MOFs due to their strong coordination ability and flexible coordination modes. In this work, three novel complexes (Pb(MCTCA)(H2O) (1), Co(HMCTCA)2(H2O)2 (2) and Cu(HMCTCA)2(H2O)2 (3)) based on the H2MCTCA ligand (5-methyl-1-(4-carboxyl)-1H-1,2,3-triazole-4-carboxylic acid) were successfully synthesized under hydrothermal conditions, respectively. X-ray single crystal structure analysis shows that complex 1 is a 3D network structure, where the central metal Pb(II) is six coordinated to form deformed triangular prism geometry. The complexes 2 and 3 are both 2D layer supramolecular structures connected through intermolecular hydrogen, where the central metals (Co/Cu) are six coordinated to form octahedral configuration geometry. Based on functional properties, it is found that complex 1 exhibits excellent detection ability for small-molecule drugs (azithromycin, colchicine and balsalazide disodium) and actinide cations (Th4+ and UO22+) within a lower concentration range without interference from other components. In particular, the detection limits of three small-molecule drugs are all lower than 0.30 μM. In addition, complexes 2 and 3 exhibited excellent catalytic reduction performance toward p-nitrophenol (PNP), with a reduction efficiency exceeding 98%. These experimental results evidence that complexes 1–3 have potential application prospects in fluorescence sensing and catalytic reduction.
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高影响因子
JOURNAL OF CATALYSIS
·
2026
·
IF 6
Zeyu Wang,Huijuan Shao,Ai Zhang,Ying Zhang,Chen Luo,Tao Jiang,Yating Wang
Porous organic polymers (POPs) are promising heterogeneous catalyst supports. However, their application in ethylene tetramerization for high-value 1-octene (1-C 8 ) is limited by nonuniform metal coordination and poorly controlled pore-confined reactions. Here, one-step solvent thermal polymerization was carried out by vinyl functionalized full diphosphine (PNP) ligand to synthesize POPs derived from the PNP ligand and used as a support for chromium-based catalysts. The characterization confirms that the interaction between POPs, modified methylaluminoxane (MMAO) and Cr(III) chloride tetrahydrofuran complex promotes the formation of Cr(III) active sites, and the chemical coordination environment of the support determines the concentration of these Cr(III) species. The adjustable POPs framework can selectively produce linear alpha-olefins (C 4 , C 6 and C 8 ) with different carbon numbers. Notably, POP-2, which exhibited a larger pore size, lower steric hindrance and a higher density of Cr(III) active sites, showed exceptional catalytic performance in the ethylene tetramerization reaction under 1 MPa and 45℃ conditions, achieving 51.54% of C 8 selectivity (1-C 8 accounted for 97.6%), C 6 /C 8 total selectivity of 88.11%, and high catalytic activity of 8.08 × 10 5 g(mol·Cr) −1 h −1 . Whereas the high-steric-hindrance POP-3 system is predisposed to trimerization. The calculation of density functional theory (DFT) revealed that the tetramerization pathway is energetically preferred over the trimerization pathway in the POPs/Cr(III) system. These results further clarified that product carbon number distribution is dually governed by the Gibbs free energy barriers of trimerization/tetramerization and the steric hindrance of Cr(III) active centers. Collectively, these findings highlight the remarkable application potential of POPs as tunable matrices for engineering Cr(III) sites and fabricating high-selectivity ethylene oligomerization catalysts.
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JOURNAL OF MOLECULAR LIQUIDS
·
2019
·
IF 4.561
Hongwei Luo,Yaoyao Zhao,Dongqin He,Qing Ji,Ying Cheng,Daoyong Zhang,Xiangliang Pan
Fe@Fe 2 O 3 core-shell nanowire is a promising heterogeneous Fenton iron catalyst to degrade organic pollutants. So far, the roles of hydroxylamine (HA) in Fe@Fe 2 O 3 /HA system for pollutant degradation still remain unknown. In this study, the HA-facilitated degradation of rhodamine B (RhB) and p-nitrophenol (PNP) by Fe@Fe 2 O 3 was reported and the underlying mechanisms were explored. Results show that addition of HA significantly enhanced degradation of organic pollutants and a higher HA dosage caused a faster degradation rate . The degradation process was completely inhibited by scavengers, indicating the hydroxyl radical (HO ) from bulk solution dominated the reactions. HA in the Fe@Fe 2 O 3 /H 2 O 2 /HA system was highly efficient to promote the generation of HO by accelerating both the Fe 3+ /Fe 2+ cycle and the H 2 O 2 decomposition. Meanwhile, HA itself was rapidly decomposed along with the pollutants degradation. About 50.5% of RhB and 46.4% of PNP were mineralized in the presence of HA. The effective pH value for degradation was expanded from 4.0 to 5.0. The EE/O calculations demonstrate that a higher energy input for PNP was required than that for RhB. This study will shed lights on the reactivity of the Fe@Fe 2 O 3 /HA system and provide an alternative pathway for removal of organic contaminants.
研究领域:
环境科学
·
化学
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2018
·
IF 2.891
Guangshan Zhang,Limin Hu,Renbo Zhao,Rongjun Su,Qiao Wang,Peng Wang
In this paper, ZnNiAl-layered double hydroxide (LDH) photocatalysts were successfully prepared using a facile and timesaving microwave-assisted method. ZnNiAl-layered double oxides (LDOs) were then achieved from ZnNiAl-LDHs photocatalyst with calcination treatment. As a control, the corresponding photocatalysts were synthesized using a traditional hydrothermal method. A set of characterization technologies including XRD, SEM, FT-IR, and N 2 adsorption was carried out to investigate the physical and chemical properties of the prepared photocatalysts. The photocatalytic activities were evaluated by the degradation of p-nitrophenol (PNP) under visible-light irradiation. Moreover, the influences of calcination temperature, photocatalyst dosage, and initial PNP concentration were also explored in this system. The results indicated that the sample transformed from LDH to LDO after 700 ○ C calcination treatment and the prepared LDO showed an outstanding photocatalytic activity. When the photocatalyst dosage was 1.0 g·L −1 and initial PNP concentration was 10 mg·L −1 , PNP removal efficiency was as high as 93.0% within 180 min under visible-light irradiation. After six cycles, the newly designed photocatalyst showed a good stability and reusability. This study shares a new preparation method for ZnNiAl-LDO as a novel photocatalyst with high efficiency for wastewater treatment.
研究领域:
环境科学
·
材料科学
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Hui Xia,Jungang Guo,Yuesuo Yang,Yuanyuan Wang,Zhongchang Wang,Xin Wang,Wenjing Zhang
Calcium peroxide (CP, CaO 2 ), acting as a source of H 2 O 2 , was combined with Fe(II) to provide a novel modified Fenton system. The removal of p- nitrophenol (PNP) in groundwater as a model pollutant was investigated using this system while addressing effect of reagents on water quality, mechanism of reactive oxygen species formation, possible degradation pathways, impact of geochemistry and process parameters on the removal efficiency. The dissolved oxygen, oxidation-reduction potential, pH, electrical conductivity and H 2 O 2 concentration in groundwater were all increased significantly due to the addition of CaO 2 and Fe(II), especially in the early stage and under acidic conditions. Within 30 min, 96% of an initial 40 mg/L PNP contamination was removed using the optimum conditions, consisting of 250 mg/L CaO 2 , 50 mg/L Fe(II), an initial pH of 2.6, oscillation frequency of 170 rpm and temperature of 298 K. The batch experiments revealed that the initial pH and the Fe(II) and CaO 2 concentrations all decisively affected removal efficiency, while the groundwater dynamics, temperature and illumination conditions had little effect. The presence of hydroxyl radicals (∙OH) and singlet oxygen ( 1 O 2 ) was confirmed by electron paramagnetic resonance spectroscopy. In addition, ∙OH quenching experiments indicated that the former rather than the latter played a major role in PNP removal. The generation of 1 O 2 in this system was also predicted by classical molecular orbital theory. These findings would provide useful technical support for the remediation of groundwater contamination .
研究领域:
环境科学
·
化学工程
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PROGRESS IN ORGANIC COATINGS
·
2025
·
IF 7.3
Mengtong Wang,Ying Miao,Rikun Liu,Liang Shen,Yingying Du,Changqing Fu
The use of bisphenol A (BPA) in traditional waterborne epoxy coating formulations is harmful to human health, and the low toughness of the cured film severely limits its application in many areas. Most BPA alternatives enhance the toughness of the epoxy cured film but compromise the coating's properties to varying degrees. Therefore, developing a BPA alternative that toughens epoxy resins without sacrificing modulus and mechanical strength remains a significant challenge. In this study, we synthesized dicarboxylic acid compound (PNP) with a structure similar to BPA, using phthalic anhydride and neopentyl glycol. This compound serves as a substitute for BPA. We systematically explored the influence of different PNP contents on the performance of waterborne epoxy resins and coatings. The results showed that PNP is more conducive to preparing waterborne epoxy resins with smaller particle sizes and stable heat storage. Compared with BPA-modified epoxy resin, PNP significantly increases the elongation at break and tensile strength of the cured film. Moreover, different PNP contents can significantly improve the coating's impact resistance, pull-off adhesion, water resistance, salt spray resistance, and acid resistance without affecting other mechanical properties and alkali resistance. This study provides a new perspective for preparing environmentally friendly, high-performance, tough, and stable waterborne epoxy coatings.
研究领域:
材料科学
·
高分子化学
·
涂层技术
·
环境科学
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ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Jingda Zhao,Xin Wang,Yubing Xu,Yuzhu Pan,Yuwei Li,Jing Chen,Qing Li,Xiaobing Zhang,Zhuoya Zhu,Zhiwei Zhao,Elias Emeka Elemike,Damian C. Onwudiwe,Byung Seong Bae,Suhaidi Bin Shafie,Wei Lei
Dual-mode photodetectors (PDs) have attracted increasing interest owing to their potential optoelectrical applications. However, the widespread use of PDs is still limited by the high cost of epitaxial semiconductors. In contrast, the solution processability and wide spectral tunability of perovskites have led to the development of various inexpensive and high-performance optoelectronic devices. In this study, we develop a high-performance electronically modulated dual-mode PD with near-infrared (NIR) narrowband and visible light broadband detection based on organic–inorganic hybrid methylammonium lead halide perovskite (MAPbX3; MA = CH3NH3 and X = Cl, Br, and I) single crystals with a pnp configuration. The operating mode of the dual-mode PD can be switched according to voltage bias polarity because the photon absorption region and carrier transport performance are tuned at different bias voltages. The dual-mode PD exhibits a NIR light responsivity of 0.244 A/W and a narrow full width at half-maximum of ∼12 nm at 820 nm at positive voltages and an average visible light responsivity of ∼0.13 A/W at negative voltages. The detectivities of both modes are high (∼1012 Jones), and the linear dynamic range is wide (>100 dB). Our study provides a new method for fabricating multifunctional PDs and can expand their application in integrated imaging systems.
研究领域:
光电技术
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材料科学
·
半导体物理
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MATERIALS RESEARCH BULLETIN
·
2024
·
IF 5.3
Fei Wang,Chen Li,Yaqian Li,Xiao Wei,Mengwei Yan,Jiaqi Wang,Yue Gao,Jiali Liu,Yixue Wang
How to manage the potential environmental pollution of waste biomass while realizing the resource utilization of the waste is a topic worthy of in-depth investigation. In this paper, after successfully preparing a deep eutectic solvents, we constructed N, Cl-CDs fluorescent probes with high fluorescence yield and biocompatibility by utilizing waste soybean residue as a cheap nitrogen-rich carbon-sourced biomass precursor. The results showed that the fluorescence quenching of N, Cl-CDs has a good linear relationship with the concentration of p-nitrophenol in the range of 0.1–60 μM, with the detection limit of 30 nM, and the fluorescence quenching mechanism was the inner filter effect. This paper demonstrates that the carbon dots fluorescence system has a superior prospect for the highly selective detection of p-nitrophenol, and provides a reliable basis for the future exploration of efficient and environmentally friendly carbon dots synthetic method as well as the economic recycling of waste.
研究领域:
环境科学
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材料科学
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生物医学
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高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2022
·
IF 8.025
Mengya Ma,Xiaobin Liu,Chaoqun Ma,Ruyue Guo,Xueling Zhang,Zhenzhong Zhang,Xueling Ren
Improved curative effects with reduced toxicity has always been the ultimate goal of gene delivery vectors for tumor immunotherapy. Panax notoginseng polysaccharide (PNP), a natural plant-derived macromolecule, not only has antitumor immune activity but also has the typical structural characteristics useful for gene delivery. In this work, positively charged polyethyleneimine (PEI) was directly grafted to the backbone of PNP to induced its charge reversal and generate a functional gene vector (PNP-PEI). Moreover, a short hairpin RNA targeting the programmed death-ligand 1 (PD-L1) was loaded into PNP-PEI to generate a potentially therapeutic nanoparticle (PNP-PEI/shPD-L1). In vitro and in vivo experiments demonstrated that PNP-PEI could efficiently carry the therapeutic shPD-L1 into tumor cells and that PNP-PEI/shPD-L1 could significantly inhibit the expression of PD-L1 and growth of B16-F10 cells. Noteworthily, treatment with PNP-PEI reversed the phenotype of macrophages from M2 to M1 subtype and promoted dendritic cell maturation, which encouraged the host immunity and enhanced the therapeutic antitumor effects. In summary, this study describes a PNP-based gene delivery vector and highlights the beneficial immunopotentiating therapeutic outcomes of PNP-PEI for tumor immunotherapy.
研究领域:
癌症免疫疗法
·
基因治疗
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药学
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分子生物学
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免疫学
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Analytical Methods
·
2015
·Vol. 7
·期 23
·9984-9991
·
IF 1.821
Qingming Zhang,Xue Li,Bingchen Li,Huanshun Yin,Shiyun Ai
A sensitive and selective electrochemical biosensor was fabricated for polynucleotide kinase (PNK) activity assay and inhibitor screening based on phos-tag-biotin mediated double signal amplification, where streptavidin and alkaline phosphatase-conjugated biotin (biotin-ALP) were used as the signal amplification units. After the immobilization of probe DNA on the electrode surface, it was hybridized with complementary DNA containing the 5′-OH terminal, the OH can be phosphorylated under the catalytic effect of PNK in the presence of ATP. The generated phosphate group at the 5′-terminal can be further recognized by phos-tag-biotin, where phos-tag-biotin was not only used as the specific recognition reagent for the phosphate group, but also the capture reagent for streptavidin to induce the further assembly of biotin-ALP. Under the catalytic effect of ALP, the substrate of p-nitrophenyl phosphate disodium salt hexahydrate (PNPP) can be hydrolyzed to produce p-nitrophenol (PNP). According to the relationship between the electrochemical response of PNP and the logarithmic value of PNK concentration, a linear range of 0.01–5 units per mL and a low detection limit of 0.0027 unit per mL were achieved. The developed method showed high selectivity. The inhibition effect of (NH4)2SO4 and Na2HPO4 was also evaluated and the IC50 values were calculated.
研究领域:
生物化学
·
分析化学
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电化学
·
分子生物学
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高影响因子
JOURNAL OF CHROMATOGRAPHY A
·
2023
·
IF 4.1
Wen Li,Xinyue Cui,Zilin Chen
An online capillary electrophoresis method based-lipase immobilized enzyme microreactor was developed for lipase kinetic study and inhibitor screening from compounds from natural products. Zeolitic Imidazolate Framework-8 (ZIF-8) has the advantages of large pore size, mild synthesis conditions and good biocompatibility. Lipase was immobilized on the inner wall of capillary with the help of the metal-organic framework ZIF-8. The results of electron microscopy showed that lipase could be aggregated and fixed on the inner wall of capillary by ZIF-8. After the experimental conditions including electrophoretic separation and enzymatic reaction were optimized, the baseline separation of substrate p-nitrophenyl acetate (pNPA) and product p-nitrophenol (pNP) was achieved within 3 min. The immobilized enzyme microreactor showed good repeatability and stability, and the determined Michaelis-Menten constant ( K m ) of lipase was 2.75 mM, which was lower than the kinetic constant determined in off-line reaction, indicating that the immobilized enzyme had a high affinity with the substrate. In addition, the IC 50 value of the positive control compound orlistat on lipase inhibition was 7.26 nM, which was consistent with the literature. Then the inhibitory activity of 10 compounds from natural products on lipase was evaluated by the ZIF-8-IMER. Among them, 7 compounds including baicalein, luteolin, epicatechin gallic acid, and chlorogenic acid, had a certain inhibitory effect on lipase. The molecular docking technology proved the interaction between the enzyme and the screened inhibitor, which provides a new method for the screening of lipase inhibitors.
研究领域:
生物化学
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分析化学
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药学
·
酶学
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高影响因子
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