CHEMICO-BIOLOGICAL INTERACTIONS
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2022
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IF 5.168
Weiwei Li,Ting Cheng,Tingting Jiang,Mengyue Zhou,Bowen Gong,Guode Zhao,Jing Li,Rong Tan,Xiaojing Yang,Kandarp Joshi,Ying Peng,Maosheng Cheng,Ting Liu,Dan Ohtan Wang,Jiang Zheng
Pyrrolizidine alkaloids (PAs) are among the most significant hepatotoxins widely distributed in plant species. Incidence of liver injuries caused by PAs has been reported worldwide, and the reactive metabolites of PAs are known to play a critical role in causing the hepatotoxicity. To better understand the toxicity-induction mechanisms, we explored the interactions of PA metabolites with cellular RNA molecules, and examined their effects on the biochemical and metabolic properties of hepatic RNAs. After exposure to retrorsine, adduction on adenosine and guanosine were detected in mouse liver microsomal incubations, cultured mouse primary hepatocytes, and mouse liver tissues. NMR analysis showed that the exocyclic amino group participated in the adduction. We found drastically altered properties and metabolism of the adducted RNA such as reverse-transcriptability, translatability, and RNase-susceptibility. In addition, endogenous modification of N 6 -methyladenosine (m6A) was remarkably reduced.
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JOURNAL OF CHROMATOGRAPHY A
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2022
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IF 4.601
Shitao Feng,An Zhang,Fengshou Wu,Xiaogang Luo,Juan Zhang
This study constructed boronic acid grafted Zr-MOF (BA-Zr-MOF) by a simple pre-installation strategy through mixed organic ligands. Typically, BA-Zr-MOF was prepared by one-step hydrothermal method used for enrichment of cis -diol-containing nucleosides through pipette tip solid-phase extraction (PT-SPE) followed by detection of high-performance liquid chromatography. It is worth mentioning that BA is well assembled into MOF and cis -diol-containing compounds can be efficiently and selectively enriched by abundant boronic acid groups. Three groups of different types of compounds were used to evaluate their selectivity and the results showed the excellent selectivity to cis -diol-containing compounds of as-prepared adsorbent. The BA-Zr-MOF adsorbent possesses a high adsorption capacity, which can reach 86.40 mg g −1 for adenosine. Under the optimal extraction condition, a PT-SPE-HPLC method based on BA-Zr-MOF for analysis of nucleosides was established. The linear range of the four nucleosides is 0.01 to 50 µg mL −1 with R 2 ≥ 0.99 and the detection limits (LODs) are estimated at between 0.005-0.012 µg mL −1 . The recoveries in urine were used to test the reliability of the analytical methods, which ranged from 82.8% to 117.1%, with intra-day relative standard deviations (RSDs) ranged from 0.1% to 4.2% and the inter-day RSDs ranged from 0.2% to 6.2%. All the results show that the pre-installation strategy based on dual ligands is an alternative to fabricate MOF composite material and BA-Zr-MOF is a promising material for the analysis of cis -diol-containing biomolecules.
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Journal of Pharmaceutical Analysis
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2022
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IF 14.026
Qiqin Wang,Lingjue Sun,Huihui Wu,Ning Deng,Xianglong Zhao,Jingwei Zhou,Tingting Zhang,Hai Han,Zhengjin Jiang
Zwitterionic sulfobetaine-based monolithic stationary phases have attracted increasing attention for their use in hydrophilic interaction chromatography. In this study, a novel hydrophilic polymeric monolith was fabricated through photo-initiated copolymerization of 3-(3-vinyl-1-imidazolio)-1-propanesulfonate (SBVI) with pentaerythritol triacrylate using methanol and tetrahydrofuran as the porogenic system. Notably, the duration for the preparation of this novel monolith was as little as 5 min, which was significantly shorter than that required for previously reported sulfobetaine-based monoliths prepared via conventional thermally initiated copolymerization. Moreover, these monoliths showed good morphology, permeability, porosity (62.4%), mechanical strength (over 15 MPa), column efficiency (51,230 plates/m), and reproducibility (relative standard deviations for all analytes were lower than 4.6%). Mechanistic studies indicated that strong hydrophilic and negative electrostatic interactions might be responsible for the retention of polar analytes on the zwitterionic SBVI-based monolith. In particular, the resulting monolith exhibited good anti-protein adhesion ability and low nonspecific protein adsorption. These excellent features seem to favor its application in bioanalysis. Therefore, the novel zwitterionic sulfobetaine-based monolith was successfully employed for the highly selective separation of small bioactive compounds and the efficient enrichment of N -glycopeptides from complex samples. In this study, we prepared a novel zwitterionic sulfobetaine-based monolith with good performance and developed a simpler and faster method for preparation of zwitterionic monoliths.
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JOURNAL OF CHROMATOGRAPHY A
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2022
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IF 4.601
Yao Sun,Zhi'an Sun,Chaozhan Wang,Yinmao Wei
Aromatic phase, as one type of reversed-phase stationary phases, shows complementary selectivity to the n -alkyl counterparts especially for certain challenging separation tasks. However, effect of phenyl numbers in aromatic ligands on retention behaviors has rarely been addressed compared with the alkyl stationary phases. To illustrate the issue, a series of polyphenyl stationary phases were facially prepared via the coupling chemistry of isocyanate with amine, including aniline (π 1 ), 4-aminobiphenyl (π 2 ), 4-amino- p -terphenyl (π 3 ) and [1,1′:4′,1′':4′',1′''-quaterphenyl]-4-amine (π 4 ), respectively. The chromatographic behaviors of the new stationary phases as well as the traditional C18 were systematically compared in terms of retention mode, hydrophobic and aromatic selectivity, shape selectivity and π-π interaction by various analytes, including alkylbenzenes , polycyclic aromatic hydrocarbons congeners and substituted benzenes with electron-withdrawing groups. Due to the homologous structure of four polyphenyl ligands, the hydrophobic selectivity, aromatic selectivity and shape selectivity of stationary phases increase with phenyl numbers in the bonded polyphenyl ligands, whereas the increment becomes insignificant from U-π 3 to U-π 4 . This phenomenon is explained by the insertion degree of analytes in the polyphenyl ligand brushes. Compared with the homemade C18, the polyphenyl phases indicate insignificant changes of shape selectivity with temperature. Notably, the new polyphenyl phases demonstrate the great selective separation towards the electron-deficient compounds through the π-π interaction. These findings make up for the understanding of the retention behavior of aromatic stationary phases.
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JOURNAL OF CHROMATOGRAPHY A
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2022
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IF 4.601
Yan Wu,Kaixing Luo,Yanjuan Liu,Wei Chen,Zhengwu Bai,Sheng Tang
Developing a versatile stationary phase to achieve the purpose of efficiently separating various target analytes is of great significance. In this work, ureido/dodecyl dual-functionalized silica (Sil-Ur-DD) was synthesized and employed as a new mixed-mode stationary phase for high-resolution chromatographic analysis. It was observed that multiple interactions, including hydrophobic, hydrophilic, hydrogen bonding, electrostatic and π-π interactions, contributed to the retention. Nucleosides and nucleobases could be effectively determined in hydrophilic interaction chromatography mode, and the separation performance of the Sil-Ur-DD was found to be even superior to that of the commercial XAmide column. Environmental endocrine disruptors, including alkylphenols, bisphenols, steroid hormones and phthalates, were more favorably separated in reversed-phase chromatography mode with highly aqueous mobile phases compared with the commercial C18-silica column. The experimental results indicated that the combined effect of ureido and long-chain alkyl groups obviously enhanced separation efficiency and selectivity. More significantly, the proposed method concerning the preparation of an efficient separation material with powerful separation ability is economical and environmentally friendly, which provides a proven and effective way for the recycling and utilization of the discarded chromatographic packing materials, thereby showing a good application prospect.
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JOURNAL OF CHROMATOGRAPHY A
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2022
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IF 4.601
Chao Fan,Jia Chen,Hui Li,Kaijun Quan,Hongdeng Qiu
Two new hydrophilic-hydrophobic and acid-base balanced liquid chromatographic stationary phases were obtained by using two long-chain monomers including undecylenic acid (UA) and oleic acid (OA) combined with short-chain 4-vinyl pyridine (Py) in-situ polymerized on silica microspheres surfaces, respectively. These two stationary phases can be used for reversed-phase liquid chromatography (RPLC) and hydrophilic interaction liquid chromatography (HILIC) modes. Hydrophilic, hydrophobic, acidic and basic analytes can be separated on two new stationary phases in RPLC or HILIC mode. Compared with commercial hydrophobic C18 columns and other HILIC columns, two new stationary phases have excellent selectivity and separation performance in the separation of 9 polycyclic aromatic hydrocarbons, 10 aromatic acids, 10 anilines and 5 oxazolidinones, respectively. This novel polymer-functionalized silica design strategy has opened up new ideas for the future of mixed-mode stationary phases with multiple functions and specificity.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Lingjue Sun,Dongsheng Xu,Yuan Shen,Jacques Crommen,Qiqin Wang,Zhengjin Jiang
Zwitterionic super-hydrophilic polymeric monoliths showed fascinating attributes because of their excellent biocompatibility, hydrophilicity, and antifouling properties. However, their commercial developments are limited by their tedious preparation process and unsatisfactory performance. 1-Carboxy- N -methyl- N -di(2-methacryloyloxyethyl)methanaminium inner salt (CBMAX), an important zwitterionic functional monomer , which exhibits excellent hydrophilicity and extremely low protein adsorption from undiluted serum. However, no carboxybetaine based monolith has been reported to date. In this study, a rapid photo-assisted generation strategy based on a sole-monomer system (CBMAX being simultaneously used as monomer and crosslinker) was proposed for preparing versatile hyper-crosslinked zwitterionic carboxybetaine polymers in capillaries within only 5 min. It is significantly faster than the conventional sole-monomer (1 h) and multi-monomer system (over 12 h) via thermally-initiated polymerization approach. Moreover, a high column efficiency of 82,000 plates/m, abundant electrostatic and hydrophilic interactions were achieved on the novel monolith due to the unique advantages of carboxybetaine. These excellent features were beneficial for the high-performance separation of various bioactive compounds (including nucleotide bases, phenols, benzoic acid and its derivatives, urea and allantoin) on this monolith. It is worth noting that this zwitterionic monolith exhibited good anti-protein adsorption ability as well as excellent enrichment capacity for N -glycopeptides from hIgG tryptic digest. In summary, the proposed photo-assisted generation strategy based on sole-monomer CBMAX is very successful and opens up a promising solution for the commercial development of zwitterionic super-hydrophilic polymeric monoliths.
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PHYTOMEDICINE
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2023
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IF 7.9
Jiana Du,Na Wang,Dehong Yu,Pei He,Yu Gao,Yanbei Tu,Yanfang Li
Background : Hyperuricemia (HUA) is a metabolic disease characterized by a high level of uric acid (UA). The extensive historical application of traditional Chinese medicine (TCM) offers a range of herbs and prescriptions used for the treatment of HUA-related disorders. However, the core herbs in the prescriptions and their mechanisms have not been sufficiently explained. Purpose : Our current investigation aimed to estimate the anti-HUA effect and mechanisms of Paeonia veitchii Lynch, an herb with high use frequency identified from data mining of TCM prescriptions. Methods : Prescriptions for HUA/gout treatment were statistically analyzed through a data mining approach to determine the common nature and use frequency of their composition herbs. The chemical constituents of Paeonia veitchii extract (PVE) were analyzed by UPLC-QTOF-MS/MS, while its UA-lowering effect was further evaluated in adenosine-induced liver cells and potassium oxonate (PO) and hypoxanthine (HX)-induced HUA mice. Results : A total of 225 prescriptions involving 246 herbs were sorted out. The properties, flavors and meridians of the appearing herbs were mainly cold, bitter and liver, respectively, while their efficacy was primarily concentrated on clearing heat and dispelling wind. Further usage frequency analysis yielded the top 20 most commonly used herbs, in which PVE presented significant inhibitory activity (IC 50 = 131.33 µg/mL) against xanthine oxidase (XOD), and its constituents showed strong binding with XOD in a molecular docking study and further were experimentally validated through XOD enzymatic inhibition and surface plasmon resonance (SPR). PVE (50 to 200 μg/mL) dose-dependently decreased UA levels by inhibiting XOD expression and activity in BRL 3A liver cells. In HUA mice, oral administration of PVE exhibited a significant UA-lowering effect, which was attributed to the reduction of UA production by inhibiting XOD activity and expression, as well as the enhancement of UA excretion by regulating renal urate transporters (URAT1, GLUT9, OAT1 and ABCG2). Noticeably, all doses of PVE treatment did not cause any liver injury, and displayed a renal protective effect. Conclusions : Our results first comprehensively clarified the therapeutic effect and mechanisms of PVE against HUA through suppressing UA production and promoting UA excretion with hepatic and renal protection, suggesting that PVE could be a promising UA-lowering candidate with a desirable safety profile for the treatment of HUA and prevention of gout.
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SENSORS AND ACTUATORS B-CHEMICAL
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2023
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IF 8.4
Yurong Bai,Mei Xiang,Zhenhua Zhou,Zhiqiang Mao,Fan Zhang
Adenosine triphosphate (ATP) is an important purine molecule. It widely exists in cells and is closely related to a variety of significant physiological and pathological processes, such as energy metabolism, respiratory regulation, inflammation, and so forth. In vivo, ATP not only provides energy for organisms at the molecular level but also activates intracellular ion channels and regulates signaling pathways. Therefore, it is of great significance to construct ATP-responsive nanochannels for understanding complex biological processes. In this work, we designed and fabricated multi-amino conjugated rhodamine B (NH 2 -RhB) functionalized artificial nanochannels, which exhibited high performance for ATP response with current and fluorescence dual signals. Significantly, owing to the non-covalent bonding of NH 2 -RhB and ATP, the system performed reversible properties for regulating ion transport and behaved as an ionic gate that can flexibly switch between the "on" and "off" state under the condition of ATP and pH. The platform showed high selectivity for ATP and the detection limit can be as low as 48.2 fM. Moreover, finite-element theoretical simulation was employed to reveal the mechanism of ATP-activated nanochannel regulating ion flux. It proved that the surface charge density of the NH 2 -RhB functionalized nanochannels can be regulated by dealing with ATP and pH. This work shows promising applications of biomimetic nanochannel with gating properties and offers prospects for the development of biosensing, nanodevice, and nanofluidic logic gates .
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Analytical Methods
·
2023
·Vol. 15
·期 47
·6571-6582
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IF 3.1
Yan Li,Xiaofan Tang,Yinhai Li,Weilong Zhao,Shengwei Guo,Chunmiao Bo
In this study, a developed chromatographic stationary phase combines the high selectivity of mixed-mode retention with a temperature-responsive property to boost separation efficiency. Copolymer brushes were grafted onto silica gels through surface initiated-atom transfer radical polymerization by polymerizing two types of monomer, temperature-responsive vinylcaprolactam (VCl) and quinine (Qun) containing benzopyridine, a tertiary ammonium positive center, and hydroxyl groups. The obtained silica@poly(Qun-co-VCl) stationary phases were packed as a chromatographic column, and the retention behavior of hydrophobic polycyclic aromatics, highly polar nucleosides, charged organic acids and β-agonists was studied for this column under different separation modes. The ability to separate different types of analyte shows that the silica@poly(Qun-co-VCl) column provides multiple hydrophobic, hydrophilic and electrostatic interactions toward analytes, achieving the separation of various compounds in one column. In addition, temperature-dependent resolution of polycyclic aromatics, nucleosides, organic acids and β-agonists was investigated using modulation of the column temperature, and the column exhibited adjustable separation selectivity by simply changing the column temperature. These results demonstrate that the grafting of copolymer brushes on a silica surface, consisting of temperature-responsive poly-VCl and multifunctional groups of poly-Qun, is useful as a mixed-mode chromatographic stationary phase for thermally-modulated multiple interactions. Additionally, this column was also used for the quantitative detection of uridine and inosine from cordyceps.
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SENSORS AND ACTUATORS B-CHEMICAL
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2023
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IF 8.4
Mengke Wang,Yaqing Han,Rui Huang,Zhonghao Wang,Guannan Wang
Fluorescent gold nanoclusters (AuNCs) have generated significant research interest because of their fascinating physicochemical properties . However, their biosensing applications are limited by the relatively low quantum yield (QY). Herein, a simple confinement effect based on AuNCs as guest molecules and Zn-containing hydroxy double salt (HDS) as host material (AuNCs@HDS) was used to significantly improve the fluorescence properties of AuNCs. The QY increased from 1.24 % to 22.80 %, and the time-tedious preparation or purification procedures were avoided. Further, the validated excellent fluorescence properties of AuNCs enabled the construction of a versatile fluorescent sensing strategy for bio-enzymes for the first time. The p-nitrophenol (pNP), a product of many bio-enzymes-catalyzed hydrolyzes of pNP-substrate, can effectively quench the fluorescence of AuNCs@HDS through an inner filter effect (IFE) process. Therefore, the AuNCs@HDS successfully detected several enzymatic disease biomarkers with robust analysis capabilities by varying the pNP-substrate, including alkaline phosphatase (ALP), β-glucosidase (β-GLU) and β-galactosidase (β-GAL). This study will inspire the design of highly fluorescent AuNCs as tools for biosensing.
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Analytical Methods
·
2023
·Vol. 15
·期 45
·6286-6293
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IF 3.1
Yali Yang,Yan Li,Zelong Long,Lingling Han,Kaijun Quan,Jia Chen,Xiuhui Liu,Hongdeng Qiu
A novel C4-modified bipyridinium stationary phase (Sil-DPC4) was prepared and characterized by elemental analysis (EA) and Fourier transform infrared spectrometry (FT-IR) and further investigated for multi-mode liquid chromatography. The chromatographic performances of Sil-DPC4 were evaluated by reversed-phase chromatography using polycyclic aromatic hydrocarbons (PAHs), phenylamines and phenols, hydrophilic interaction chromatography using nucleosides and nucleobases, and ion exchange chromatography using inorganic ions and organic ions. The effects of the acetonitrile content, salt concentration and pH value of the mobile phase on the retention of Sil-DPC4 were also investigated. Sil-DPC4 showed multiple retention mechanisms including π–π, hydrophobic and electrostatic interactions for PAHs, phenylamines and phenols compared with a dipyridine modified silica stationary phase (Sil-DP) and C18 in RPLC, faster separation for nucleosides and nucleobases compared with Sil-DP, and higher hydrophilicity than HILIC in HILIC, and stronger retention and better separation ability for inorganic ions and organic ions in comparison to Sil-DP in IEC. Besides, Sil-DPC4 was used successfully to detect iodide in artificial seawater and had the potential to analyze radionuclide iodine-131 in seawater. In conclusion, multiple retention mechanisms of Sil-DPC4 could make it have potential applications in complex samples.
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