Inorganic Chemistry Frontiers
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2021
·Vol. 8
·期 10
·2591-2602
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IF 6.569
Yuyuan Xiao,Rong Sun,Jiefeng Liang,Yuhui Fang,Zheng Liu,Shangda Jiang,Bingwu Wang,Song Gao,Wenliang Huang
Homoleptic tris(6,6′-dimethyl-2,2′-bipyridine) rare earth metal complexes M(κ2-dmbp)3 (M = Y, Tb, Dy, Ho, Er; dmbp = 6,6′-dimethyl-2,2′-bipyridine) were synthesized by in situ reduction of 3 equiv. of dmbp with excess KC8 in the presence of 1 equiv. of rare earth metal trihalides. All compounds were characterized by X-ray crystallography, UV-Vis-NIR spectroscopy, infrared (IR) spectroscopy, elemental analysis, and magnetic measurements. While the structural parameters and spectroscopic data confirmed the existence of the trivalent rare earth metal cation and three dmbp radical anions, the electron paramagnetic resonance (EPR) spectrum and the measured magnetic moment of Y(κ2-dmbp)3 indicated that two parallel dmbp radical anions were antiferromagnetically coupled. For paramagnetic rare earth metal ions, room temperature magnetic susceptibility values indicated a weak ferromagnetic interaction between the metal ion and the remaining dmbp radical. Density functional theory (DFT) calculations were performed on Y(κ2-dmbp)3 to gain insight into the electronic structures of these homoleptic metal complexes. The computational results were consistent with the structural, spectroscopic, and magnetic data for a S = 1/2 ground state and spin densities mostly residing on one dmbp radical anion, while the spins on the other two parallel dmbp radical anions being antiferromagnetically coupled.
研究领域:
化学
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材料科学
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物理化学
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CHEMISTRY & BIODIVERSITY
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2024
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IF 2.3
Lihong Chen,Zijia Zhao,Rominah Onintsoa Diarimalala,Zhongwei Chen,Yu Wang,Taozhu Zhan,Yanchao Zhao,Chunhui Ma,Xingyue Wang,Chenqi Zhao,Zicheng Xiao,Kanghong Hu,Pingfan Wu
Polyoxometalates (POMs) are promising inorganic drug candidates for cancer chemotherapy. They are becoming attractive because of their easy accessibility and low cost. Herein, we report the synthesis and antitumor activity studies of four Lindqvist-type POMs with mixed-addenda atoms Na 2 [V 4 W 2 O 16 {(OCH 2 ) 3 CR}] (R=−CH 2 OH, −CH 3 , −CH 2 CH 3 ) and (Bu 4 N) 2 [V 3 W 3 {(OCH 2 ) 3 CH 2 OOCCH 2 CH 3 }]. Compared with the current clinical applied antitumor drug 5-fluorouracil (5-FU) or Gemcitabine, analysis of MTT/CCK-8 assay, colony formation and wound healing assay revealed that the {V 4 W 2 } POMs had acceptable cytotoxicity in normal cells (293T) and significant inhibitory effects on cell proliferation and migration in three human tumor cell lines: human lung carcinoma cells (A549), human cervical carcinoma cells (HeLa), and human breast cancer cells (MCF-7). Interestingly, among the POMs analyzed, the therapeutic index (TI) of the {V 4 W 2 } POM with R= -CH 2 OH was relatively the most satisfactory. Thus, it was subsequently used for further studies. Flow cytometry analysis showed it prompted cellular apoptosis rate. qRT-PCR and Western blotting analysis indicated that multiple cell death pathways were activated including apoptosis, autophagy, necroptosis and pyroptosis during the POM-mediated antitumor process. In conclusion, our study shows that the polyoxotungstovanadate has great potential to be developed into a broad-spectrum antitumor chemotherapeutic drug. Graphical
研究领域:
化学
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药理学
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肿瘤学
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JOURNAL OF CHROMATOGRAPHY A
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2024
·
IF 3.8
Yang Zhao,Yufang Ming,Yang Yang,Changyu Cai,Yujie Bi,Qing Fu,Yanxiong Ke
In this work, a chromatographic method for the separation of carbohydrates was proposed. Tris-(hydroxymethyl)-amine (TRIS) functionalized silica-based hydrophilic interaction liquid chromatography (HILIC) stationary was synthesized. The dynamically absorbed borate layer is generated by using borate buffer as a polar modifier due to the complexation of borate with TRIS ligand in the stationary phase. The chromatographic systems were analyzed by the linear solvation energy relationship model. The calculated system constants revealed the enhancement of anionic exchange by the addition of borate in the mobile phase system. In addition, ligand exchange is critical for the retention and elution order of sugars and sugar alcohols. Carbohydrates displayed prolonged retention with different selectivity profiles relating to their complexation coefficients with borate. Experiment results showed that the effect of borate in this chromatographic system was stable within the range of pH 3–7 and borate concentration of 5–15 mM. This work provides a complementary solution for the separation of carbohydrates. It can also be extended to the separation of glycosides.
研究领域:
分析化学
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色谱学
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碳水化合物化学
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2013
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IF 2.672
Xiaoquan Lu,Li Wang,Dong Liu,Jie Du,Haifeng Wang
An interesting phenomenon that significant cathodic electrochemiluminescence of tris(2,2′-bipyridine)ruthenium(II) with assistance of metal nanoparticles (Ag, Cu) on Pt electrode was observed for the first time in acid buffer solution. This is different from that only anodic electrochemiluminescence occurs when bare Pt electrode is used. Both anodic and cathodic ECL peaks were found at 0.4 V with positive potential scan and 0 V with negative initial potential scan, respectively, in the presence of Ag. A possible mechanism was proposed that Ag might act as a co-reactant to ignite cathodic ECL of Ru ( bpy ) 3 2 + system in low pH condition, which was similar to the result we observed previously in the case of Au. Considering high market price of Au, relatively cheaper metal Ag is more promising for potential application in ECL.
研究领域:
分析化学
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材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY
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2026
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IF 9.1
Hongfen Zuo,Qilin Wei,Yingxian Wang,Yan Zhang,Genghao Gong
Rigid triphenol intercalation regulates GO nanochannels and interlayer interactions. • Pressure-assisted assembly builds compact, ordered lamellar membranes with few defects. • Optimal membrane delivers separation factor ∼ 3568 and flux of 0.67 kg·m −2 ·h −1 . • DFT calculations confirm diffusion selectivity governs separation via lower water barrier. Isopropanol (IPA) dehydration is a critical industrial process, yet it remains challenged by the energy-intensive nature of conventional distillation; however, graphene oxide (GO) membranes often suffer from the trade-off between flux and selectivity, as well as limited structural stability. Herein, a Tris-phenol-intercalated GO (TG) membrane was fabricated via a pressure-assisted filtration strategy. The rigid Tris-phenol molecules served as interlayer spacers to regulate the nanochannel structure, while their abundant hydroxyl groups enhanced water adsorption and hydrogen-bonding interactions. Meanwhile, pressure-assisted assembly promoted the formation of a compact and highly ordered lamellar architecture with well-connected transport pathways. Under the selected fabrication conditions, the TG membrane achieved a separation factor of >3.6 × 10 3 with a water flux of 0.67 kg m −2 h −1 for the dehydration of 90 wt% IPA at 60 °C, significantly outperforming the membrane prepared by conventional vacuum filtration method. First-principles calculations revealed that Tris-phenol intercalation enhanced selective water transport by lowering the diffusion energy barrier for water while maintaining a relatively high barrier for IPA, indicating that diffusion selectivity dominates the separation process. The membrane also maintains a separation factor above 6000 during 40 h of continuous operation. This work demonstrates that coupling molecular intercalation with pressure-assisted assembly is an effective strategy for constructing high-performance two-dimensional GO membranes and provides valuable guidance for the design of energy-efficient membranes for solvent dehydration. Download: Download high-res image (167KB) Download: Download full-size image
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MOLECULES
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2024
·Vol. 29
·期 24
·5887
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IF 4.2
Jiaxiang Liu,Yongwen Zhang,Ruijuan Yao,Haitao Ren,Weijie Wang,Haohao Feng,Wentao Li,Zongcheng Miao
Achieving superior circularly polarized luminescence brightness (BCPL) is an important subject and continuous challenge for chiroptical materials. Herein, by applying a binary molecular design for the synthesis of chiral organo-Tb3+molecules, a novel pair of mononuclear chiraltris-pyrazolate-Tb3+enantiomers, [Tb(PMIP)3(R,R-Ph-PyBox)] (2) and [Tb(PMIP)3(S,S-Ph-PyBox)] (5), have been synthesized and characterized. The three 1-phenyl-3-methyl-4-(isobutyryl)-5-pyrazolone (HPMIP) ligands play the role of efficient luminescence sensitizers and strong light-harvesting antennas, while the enantiopure 2,6-bis(4-phenyl-2-oxazolin-2-yl) pyridine ligand (R,R/S,S-Ph-PyBox) is employed as the strong point-chiral inducer. With the proper combination of theHPMIPandChiral-Ph-PyBoxwithin the Tb3+enantiomers, strong (PMIP)−-centered π-π*electronic absorption (ε263 nm= 38,400–39,500 M−1cm−1) and brilliant high-purity ligand-sensitized Tb3+-centered green luminescence (ΦPL= 47–48%) were observed. In addition, a clear circularly polarized luminescence (CPL) activity (|glum| = 0.096–0.103) was also observed, resulting in a strongBCPL(610–623 M−1cm−1) for the two Tb3+enantiomers from the hypersensitive transitions. Our results offer an effective path to develop high-performance chiroptical organo-Tb3+luminophores.
研究领域:
化学
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材料科学
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LUMINESCENCE
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2015
·Vol. 30
·期 8
·1269-1273
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IF 1.518
Yinggui Zhu,Lili Zou,Qin Dong,Derong Jiang
Quenching effects of bergenin, based on the electrochemiluminescence (ECL) of the tris(2,2′-bipyridyl)-ruthenium(II) (Ru(bpy) 3 2+ )/tri-n-propylamine (TPrA) system in aqueous solution, is been described. The quenching behavior can be observed with a 100-fold excess of bergenin over Ru(bpy) 3 2+ . In the presence of 0.1 m TPrA, the Stern–Volmer constant ( K SV ) of the ECL quenching is as high as 1.16 × 10 4 M −1 for bergenin. The logarithmic plot of the inhibited ECL versus logarithmic plot of the concentration of bergenin was linear over the range 3.0 × 10 −6 –1.0 × 10 −4 mol/L. The corresponding limit of detection was 6.0 × 10 −7 mol/L for bergenin (S/N = 3). In the mechanism of quenching it is believed that the competition of the active free radicals between Ru(bpy) 3 2+ /TPrA and bergenin was the key factor for the ECL inhibition of the system. Photoluminescence, cyclic voltammetry, coupled with bulk electrolysis, supports the supposition mechanism of the Ru(bpy) 3 2+ /TPrA–bergenin system. Copyright © 2015 John Wiley & Sons, Ltd.
研究领域:
分析化学
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药学
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ELECTROCHIMICA ACTA
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2022
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IF 7.336
Ping Zhou,Wenxuan Fu,Lurong Ding,Yajuan Yan,Weiliang Guo,Bin Su
Electrochemiluminescence (ECL) generation by tris(2,2’-bipyridyl)ruthenium (Ru(bpy) 3 2+ ) and S 2 O 8 2− is one of most frequently studied cathodic systems. However, the reaction mechanism is yet to be fully resolved, since the reaction involving highly reactive intermediates occurs at the negative potential limit of aqueous solutions. In this work we used bismuth microwire (BiMW) as the working electrode and ECL microscopy (ECLM) as the imaging tool to study the mechanism of cathodic ECL generation by Ru(bpy) 3 2+ /S 2 O 8 2− . Thanks to its high hydrogen evolution overpotential, BiMW electrode could provide us with a wide negative potential window in aqueous solutions. While ECLM allowed us to determine the thickness of ECL layer (TEL), which was found to vary from ca. 3.4 μm to 3.0 μm with increasing the concentration of S 2 O 8 2− . Given the chemical reduction of S 2 O 8 2− by Ru(bpy) 3 + is essential for extending the concentration profile of SO 4 •− , the slightly changed TEL is likely related to the instability of Ru(bpy) 3 + in aqueous solutions. Finally, no ECL was detected for Ru(bpy) 3 2+ -labelled microbeads, implying that S 2 O 8 2− could not work as the cathodic coreactant like tri- n -propylamine (TPrA) as the anodic one in bead-based immunoassays .
研究领域:
分析化学
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电化学
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CARBOHYDRATE POLYMERS
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2017
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IF 4.811
Miaomiao Han,Xiaosa Jin,Han Yang,Xiao Liu,Yadong Liu,Shengxiang Ji
Traditional cellulose-based chiral stationary phases (CSPs) are prepared by physically coating cellulose derivatives onto substrates and only compatible with a very limited range of solvents as the mobile phase. Therefore, chemical immobilization of cellulose derivatives onto silica gel has been efficiently applied to improve the solvent compatibility of cellulose-based CSPs. Here we developed a novel approach to homogeneously modifying cellulose tris(3,5-dimethylphenylcarbamate) (CDMPC). A series of carboxylic acid functionalized CDMPCs (CC-Xs) with controlled amounts and randomly distributed carboxylic acid groups was synthesized. CC-Xs were effectively immobilized onto amine-modified silica gel to afford immobilized CSPs. Compared to coated-type CSPs, immobilized CSPs significantly improved the solvent compatibility while maintaining similar chiral recognition abilities, but the introduction of excessive functional groups led to a deteriorated performance for columns. Moreover, a commercial drug, atenolol, was also sufficiently separated on the immobilized CSPs.
研究领域:
分析化学
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有机化学
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Chemistry Central Journal
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2013
·Vol. 7
·期 1
·1-5
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IF 1.312
Liu Run-Qiang,Bai Lian-yang,Zhang Yi-Jun,Zhang Yu-Ping
Background At present, the study on the homogeneous-phase derivatization of cellulose in ionic liquid is mainly focused on its acetylation. To the best of our knowledge, there has been no such report on the preparation of cellulose-tris(3,5-dimethylphenylcarbamate) (CDMPC) with ionic liquid 1-allyl-3-methyl-imidazolium chloride (AmimCl) so far.Results With ionic liquid 1-allyl-3-methylimidazolium chloride (AmimCl) as a reaction solvent, cellulose-tris(3,5-dimethylphenylcarbamate) (CDMPC) was synthesized by the reaction of 3,5-dimethylphenyl isocyanate and soluble microcrystalline cellulose in a homogeneous phase. The synthesized CDMPC was then coated onto the surfaces of aminopropyl silica gel to prepare a chiral stationary phase (CSP). The prepared CSP was successfully used in chiral separation of seven racemic pesticides by high performance liquid chromatography (HPLC). Good chiral separation was obtained using n-hexane and different modifiers as the mobile phases under the optimal percentage and column temperature, with the resolution of metalaxyl, diniconazole, flutriafol, paclobutrazol, hexaconazole, myclobutanil and hexythiazox of 1.73, 1.56, 1.26, 1.00, 1.18, 1.14 and 1.51, respectively. The experimental results suggested it was a good choice using a green solvent of AmimCl for cellulose functionalization.Conclusion CDMPC was successfully synthesized as the chiral selector by reacting 3, 5-dimethylphenyl isocyanate with dissolved microcrystalline cellulose in a green ionic liquid of AmimCl.
研究领域:
分析化学
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绿色化学
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ACS Applied Materials & Interfaces
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2022
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IF 10.383
Xijian Duan,Jingrui Ma,Wenda Zhang,Pai Liu,Haochen Liu,Junjie Hao,Kai Wang,Lars Samuelson,Xiao Wei Sun
InP quantum dots (QDs) are the most competitive in terms of environmentally friendly QDs. However, the synthesis of InP QDs requires breakthroughs in low-cost and safe phosphorus precursors such as tri(dimethylamino)phosphine [(DMA)3P]. It is found that even if the oxygen is completely avoided, there are still oxidation state defects at the core/shell interface of InP QDs. Herein, the record-breaking (DMA)3P-based red InP QDs were synthesized with the assist of HF processing to eliminate the InPOx defect and improve the fluorescence efficiency. The maximum photoluminescence quantum yield was 97.7%, which is the highest of the red InP QDs synthesized by the aminophosphine. The external quantum efficiency and brightness of the QD light-emitting diode device are also improved accordingly from 0.6% and 1276 cd·m–2 to 3.5% and 2355 cd·m–2, respectively.
研究领域:
材料科学
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纳米技术
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化学工程
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高影响因子
ChemistryOpen
·
2023
·Vol. 12
·期 3
·e202200259
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IF 2.3
Yulin Zhou,Jicheng Niu,Yan Zhou,Fei Li
Graphical An open liquid plasticine-based FASS system (FASS: field-amplified sample stacking) for protein enrichment was developed, with which proteins can be enriched 40–80-fold by LP-FASS within 40 min. Protein analysis is an important approach for disease diagnosis, in which sample pretreatment is an essential step since protein samples are often complex and many protein biomarkers are of low abundance. Here, given the good openness and light transmission of liquid plasticine (LP), which is a liquid entity formed by SiO 2 nanoparticles and encapsulated aqueous solution, we developed a LP-based field-amplified sample stacking (FASS) system for protein enrichment. The system was composed of a LP container, a sample solution and a Tris-HCl solution containing hydroxyethyl cellulose (HEC). The system design, mechanism investigation, optimization of experimental parameters and characterization of LP-FASS performance for protein enrichment were well studied. Under the optimized experimental conditions of 1 % HEC, 100 m m Tris-HCl and 100 V in the LP-FASS system, a 40–80 times enrichment of proteins was obtained in 40 min using bovine hemoglobin (BHb) as the model protein using the constructed LP-FASS system. The simultaneous enrichment of multiple proteins (phycocyanin, BHb and cytochrome C) was also realized using the system. The LP-FASS system can serve as a new platform for protein enrichment which is easy to be combined with online and offline detections.
研究领域:
分析化学
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蛋白质组学
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生物医学工程
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高影响因子
危险品化学品经营许可证（带存储）