Separations
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2022
·Vol. 10
·期 1
·4
·
IF 3.344
Hongmei Zhou,Junhui Zhang,Aihong Duan,Bangjin Wang,Shengming Xie,Liming Yuan
A new facile strategy was designed to prepare the phenyboronic acid-functionalized Fe3O4magnetic nanoparticles (Fe3O4@PBA) via direct silanization and thiol-ene click chemistry for the selective adsorption of ortho-dihydroxy-containing compounds. The three kinds of Fe3O4@PBA nanoparticles obtained showed excellent adsorption capacity and selectivity for ortho-dihydroxy-containing compounds including adenosine ando-dihydroxybenzene. Among them, the Fe3O4@MPS@MPBA exhibited the highest adsorption capacity and selectivity for adenosine ando-dihydroxybenzene, followed by Fe3O4@MPTES@AAPBA and Fe3O4@MPTES@VPBA. A synthesis method of superparamagnetic and boronate affinity nanocomposites with mild reaction conditions and simple process has been developed, which also provides a novel way for the synthesis of other types of enrichment materials of ortho-dihydroxy-containing compounds.Keywords:phenyboronic-acid-functionalized;Fe3O4magnetic nanoparticles;ortho-dihydroxy-containing compounds
研究领域:
化学
·
材料科学
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产品关联
DOI
高影响因子
Toxics
·
2024
·Vol. 12
·期 4
·281
·
IF 3.9
Mengtao Zhang,Jianghong Shi,Bing Li,Hui Ge,Huanyu Tao,Jiawei Zhang,Xiaoyan Li,Zongwei Cai
Dihydroxylated polybrominated diphenyl ethers (DiOH-PBDEs) could be the metabolites of PBDEs of some organisms or the natural products of certain marine bacteria and algae. OH-PBDEs may demonstrate binding affinity to thyroid hormone receptors (TRs) and can disrupt the functioning of the systems modulated by TRs. However, the thyroid hormone disruption mechanism of diOH-PBDEs remains elusive due to the absence of diOH-PBDEs standards. This investigation explores the potential disruptive effects of OH/diOH-PBDEs on thyroid hormones via competitive binding and coactivator recruitment with TRα and TRβ. At levels of 5000 nM and 25,000 nM, 6-OH-BDE-47 demonstrated significant recruitment of steroid receptor coactivator (SRC), whereas none of the diOH-PBDEs exhibited SRC recruitment within the range of 0.32–25,000 nM. AutoDock CrankPep (ADCP) simulations suggest that the conformation of SRC and TR–ligand complexes, particularly their interaction with Helix 12, rather than binding affinity, plays a pivotal role in ligand agonistic activity. 6,6′-diOH-BDE-47 displayed antagonistic activity towards both TRα and TRβ, while the antagonism of 3,5-diOH-BDE-100 for TRα and TRβ was concentration-dependent. 3,5-diOH-BDE-17 and 3,5-diOH-BDE-51 exhibited no discernible agonistic or antagonistic activities. Molecular docking analysis revealed that the binding energy of 3,3′,5-triiodo-L-thyronine (T3) surpassed that of OH/diOH-PBDEs. 3,5-diOH-BDE-100 exhibited the highest binding energy, whereas 6,6′-diOH-BDE-47 displayed the lowest. These findings suggest that the structural determinants influencing the agonistic and antagonistic activities of halogen phenols may be more intricate than previously proposed, involving factors beyond high-brominated PBDEs or hydroxyl group and bromine substitutions. It is likely that the agonistic or antagonistic propensities of OH/diOH-PBDEs are instigated by protein conformational changes rather than considerations of binding energy.
研究领域:
环境科学
·
毒理学
·
生物化学
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DOI
PubMed
高影响因子
CHEMOSPHERE
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2019
·
IF 5.108
Mengtao Zhang,Wei Guo,Juntong Wei,Jianghong Shi,Jiawei Zhang,Hui Ge,Huanyu Tao,Xiaowei Liu,Qing Hu,Zongwei Cai
Dihydroxylated polybrominated diphenyl ethers (diOH-PBDEs) can be natural products of marine organisms or the metabolites of PBDEs. The optimal determination method and concentration of diOH-PBDEs in seafood are unknown due to a lack of commercially available standards. In the present study, diOH-PBDEs were synthesized, and an efficient measurement method for OH-PBDEs and diOH-PBDEs in sea fish muscle samples, including extraction, clean-up and gas chromatography-tandem mass spectrometry (GC-MS/MS) analysis, was established. Pressurized liquid extraction (PLE) followed by partitioning with a KOH solution and florisil cartridge clean-up proved to be a reliable and robust method for detecting all OH-PBDEs/diOH-PBDEs. GC-MS/MS with an electron ionization (EI) source analysis was a sensitive analytical instrument for OH-PBDEs/diOH-PBDEs. The recovery using this method ranged from 19% to 101%, 28%–88% and 42%–90% for 10 ng, 20 ng and 40 ng spiking levels, respectively. The equipment detection limits (EDLs) were in the range of 0.31–2.78 pg/μL, and the limits of detection (LOD) for the method were in the range of 5.07–38.74 pg/g wet weight. Concentrations of diOH-PBDEs in the marine fish muscle samples were in the range of 32.43–1528.63 pg/g wet weight. Similar compositions of OH-PBDEs/diOH-PBDEs were found within the same family of marine fish.
研究领域:
环境科学
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分析化学
·
海洋生物学
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DOI
PubMed
高影响因子
PLANTA MEDICA
·
2022
·Vol. 88
·期 14
·1369-1383
·
IF 3.007
Song Mengmeng,Xu Zhuicheng,Han Sixuan,Sheng Xianjie,Chen Yan,Li Xinru,Su Yan,Li Qin,Shan Chenxiao,Xie Tong,Kang An
Agrimonia pilosa is a perennial herbaceous flowering plant, commonly known as agrimony or hairy agrimony. The dried aerial parts of this species have been widely used for the treatment of acute diarrhea, hemostasis, and other inflammation-related diseases. However, information on the in vivo metabolism of A. pilosa constituents is limited. In this study, the phytochemical profile of A. pilosa was investigated using HPLC-Q-TOF-MS/MS combined with a nontargeted diagnostic ion network analysis strategy. An information-dependent acquisition method with multiple filters was utilized to screen possible prototypes and metabolites in complex biological matrices. Furthermore, various data-processing techniques were applied to analyze possible prototypes and their metabolites in rat plasma, feces, and urine following oral administration of A. pilosa extract. A total of 62 compounds, which belonged to five main structural classes (21 phenols, 22 flavonoids, 6 coumarins, 3 triterpenes, and 10 organic acids), were tentatively identified in A. pilosa. In addition, using our proposed stepwise method, 32 prototypes and 69 metabolites were detected in rat plasma, feces, and urine. The main metabolic pathways after the oral administration of A. pilosa extract were revealed to include methylation, dihydroxylation, demethylation, hydrolysis, sulfation, and glucuronidation. This comprehensive in vivo and in vitro identification of the possible active components in A. pilosa could provide a basis for understanding its various pharmacological activities.
研究领域:
药理学
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分析化学
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代谢组学
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DOI
PubMed
高影响因子
Scientific Reports
·
2021
·Vol. 11
·期 1
·1-11
·
IF 4.38
Xue Shu-Wen,Tian Yue-Xin,Pan Jin-Cheng,Liu Ya-Ni,Ma Yan-Ling
Pseudomonas aeruginosa DN1 can efficiently utilize fluoranthene as its sole carbon source, and the initial reaction in the biodegradation process is catalyzed by a ring-hydroxylating dioxygenase (RHD). To clarify the binding interaction of RHD with fluoranthene in the strain DN1, the genes encoding alpha subunit (RS30940) and beta subunit (RS05115) of RHD were functionally characterized through multi-technique combination such as gene knockout and homology modeling as well as molecular docking analysis. The results showed that the mutants lacking the characteristic alpha subunit and/or beta subunit failed to degrade fluoranthene effectively. Based on the translated protein sequence and Ramachandran plot, 96.5% of the primary amino-acid sequences of the alpha subunit in the modeled structure of the RHD were in the permitted region, 2.3% in the allowed region, but 1.2% in the disallowed area. The catalytic mechanism mediated by key residues was proposed by the simulations of molecular docking, wherein the active site of alpha subunit constituted a triangle structure of the mononuclear iron atom and the two oxygen atoms coupled with the predicted catalytic ternary of His 217 -His 222 -Asp 372 for the dihydroxylation reaction with fluoranthene. Those amino acid residues adjacent to fluoranthene were nonpolar groups, and the C 7 -C 8 positions on the fluoranthene ring were estimated to be the best oxidation sites. The distance of C 7 -O and C 8 -O was 3.77 Å and 3.04 Å respectively, and both of them were parallel. The results of synchronous fluorescence and site-directed mutagenesis confirmed the roles of the predicted residues during catalysis. This binding interaction could enhance our understanding of the catalytic mechanism of RHDs and provide a solid foundation for further enzymatic modification.
研究领域:
微生物学
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生物化学
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分子生物学
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环境科学
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产品关联
DOI
PubMed
高影响因子
WATER RESEARCH
·
2024
·
IF 11.4
Qi Lu,Qi Han,Hongnan Liu,Li Feng,Yongze Liu,Ziwen Du,Liqiu Zhang
Dissolved black carbon (DBC) released from biochar, is an essential group in the dissolved organic matter (DOM) pool and is widely distributed in aquatic environments. In various advanced oxidation processes (AOPs), DBC exhibits enhanced free radical scavenging compared to typical DOM, attributed to its smaller molecular weight and more compacted aromatic structure; however, the molecular-level transformations of DBC in different AOPs , such as UV/H 2 O 2 , UV/PDS, and UV/Chlorine, remain unclear. This study employed a DBC derived from wheat biochar for experimentation. Characterization involved ultraviolet-visible (UV–Vis) spectroscopy and fluorescence excitation-emission-matrix (EEM) spectroscopy, revealing the transformation of DBC through diminished SUVA 254 values and reduced intensity of three-dimensional fluorescence peaks. Further insights into the transformation were gained through Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS). After each UV-AOP treatment, a conspicuous augmentation in the oxygen content of DBC was observed. The detailed oxygenation processes were elucidated through mass difference analysis, based on 23 types of typical reactions. Results indicated that oxygenation reactions were most frequently detected in all three UV-AOP treatments. Specifically, the hydroxylation (+O) predominated in UV/H 2 O 2 , while the di-hydroxylation (+2O) prevailed in UV/PDS. UV/Chlorine treatments commonly exhibited tri-hydroxylation (+3O), with the identification of 1194 Cl-BPs of unknown structures. This study contributes to a comprehensive understanding of the molecular transformations of DBC induced by various free radicals in different UV-AOP processes, leading to a better understanding of the different fates of DBC in UV-AOP processes. In addition, the identification of DBC as a precursor of by-products will also contribute to the understanding of how to inhibit the generation of by-products.
研究领域:
环境科学
·
化学工程
·
分析化学
·
水处理
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DOI
PubMed
高影响因子
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