ANALYTICAL CHEMISTRY
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2025
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IF 6.7
Jinlei Yang,Jing Wang,Runsong Cheng,Tianyi Liao,Siyuan Pan,Murong Du,Weiliang Liu,Liying Yan,Sichun Zhang,Xinrong Zhang
Single-cell metabolic analysis has not yet achieved the coverage of bulk analysis due to the diversity of cellular metabolites and the ionization competition among species. Direct ionization methods without separation lead to the masking of low-intensity species. By designing a capillary column emitter and introducing reverse-phase chromatography principles, we achieved the microseparation of lipophilic and hydrophilic metabolites and lowered the limit of detection of hydrophilic metabolites to the level of a single oocyte. We identified 517 metabolite species in a single oocyte, achieving coverage and reproducibility comparable to those of bulk analysis. By comparing oocytes at different maturation stages, 76 metabolic features were identified with significant differences between the germinal vesicle and meiosis II stages. Metabolite level changes suggested the roles of lipid metabolism remodeling, increased amino acid synthesis, and a shift from pyrimidine metabolism to purine metabolism in the process of oocyte maturation. This microseparation mass spectrometry analysis is expected to promote single-cell metabolomics.
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2024
·Vol. 25
·期 17
·9465
·
IF 4.9
Xingyun Zhao,Yifan Niu,Chengxiao Zhao,Zhenyu Li,Ke Li,Xuemei Qin
There are great challenges in the field of natural product isolation and purification and in the pharmacological study of oligosaccharide monomers. And these isolation and purification processes are still universal problems in the study of natural products (NPs), traditional Chinese medicine (TCM), omics, etc. The same polymer-modified materials designed for the special separation of oligosaccharides, named Sil-epoxy-PEI and Sil-chloropropyl-PEI, were synthesized via two different methods and characterized by scanning electron microscopy combined with energy spectrum analysis, Fourier transform infrared spectroscopy, thermogravimetric analysis, zeta potential as well as surface area analysis, etc. Several nucleotide/nucleoside molecules with different polarities and selectivities were successfully isolated in our laboratory using stainless-steel columns filled with the synthesized material. In addition, the separation of saccharide probes and oligosaccharides mixtures in water extracts of Morinda officinalis were compared in HILIC mode. The results showed that the resolution of separations for the representative analytes of the Sil-epoxy-PEI column was higher than for the Sil-chloropropyl-PEI column, and the developed stationary phase exhibited improved performance compared to hydrothermal carbon, amide columns and other HILIC materials previously reported.
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Advanced Science
·
2025
·
IF 14.1
Yating Li,Jason Tan,Yanqin Tu,Jingnan Wu,Zaifang Zhang,Yifeng Wei,Xinan Jiao,Yan Zhou
DNA base modification is a common strategy used by bacteriophages to evade host immune detection. A prominent example is dU-DNA, where thymidine is globally replaced with 2′-deoxyuridine. Despite its widespread occurrence, dU-DNA's biosynthetic pathways and functional roles remain incompletely understood. Here, different enzymes supporting dU-DNA biosynthesis in phage PBS1, Roseophage DSS3_VP1, and Yersiniophage PhiR1-37 are identified and characterized. The dU nucleotide precursor is supplied by phage dCTP deaminases (Dcds). Thymidine nucleotides are degraded by dTMP phosphatases (Dtms) in PBS1 and DSS3_VP1, and by a dTTP pyrophosphatase (Dtt) in PhiR1-37, preventing incorporation into phage DNA. The dU-DNA, isolated from Yersiniophage PhiR1-37 or synthesized by PCR, demonstrates resistance to cleavage by restriction enzymes recognizing thymidine-containing sequences, partial resistance to Lb Cas12a nuclease recognizing a TTTV PAM site, while remaining sensitive to Sp Cas9 nuclease recognizing a NGG PAM site. A phylogenetic analysis of PBS1 dCTP deaminase and closely related T4 phage dCMP deaminase suggest possible evolutionary origins from bacterial dCDP deaminases. Overall, these findings suggest independent acquisition of dU-DNA biosynthetic enzymes and pathways in the diverse phages, and support its protective function against different host-encoded nucleases.
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MICROCHEMICAL JOURNAL
·
2025
·
IF 5.1
Yansheng Liu,Haoteng Wang,Guofu Wang,Xiaobo Jia,Jin Zhou,Hongqi Li,Haixin Chang,Zhicheng Jin,Kang Li,Zhaoxu Li
Contamination with heavy metal ions is one of the most widespread and harmful sources of environmental pollution. In this work, we developed a rapid, reproducible, and highly sensitive biosensor based on the surface plasmon resonance (SPR) effect to detect mercury ions (Hg 2+ ) in DI water, tap water, and rainwater. A homemade differential phase SPR biosensor was designed and constructed, with phase shifts in the SPR interference spectrum extracted using a windowed Fourier transform (WFT) method. Custom software was developed to extract the phase shift values of the SPR system in real-time. The sensing surface of the SPR system is an Au film functionalized with thymine-1-acetic acid (T-COOH), where the thymine group specifically binds to Hg 2+ , forming a stable T-Hg 2+ -T structure. By integrating a microfluidic chip with the sensing surface, the SPR system achieves a detection limit for Hg 2+ of 8.59 × 10 −4 mg/L in DI water, 7.26 × 10 −4 mg/L in tap water, and 8.82 × 10 −4 mg/L in rainwater, with excellent specificity compared to ions like Ca 2+ , Cd 2+ , Co 2+ , Cu 2+ , Fe 2+ , Mg 2+ , and Pb 2+ . Additionally, L-cysteine is used for the regeneration of the SPR sensor, which shows no significant loss of sensitivity after 40 cycles. Therefore, the differential phase SPR biosensor holds great promise for future applications in environmental monitoring, drinking water safety, and healthcare.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Chunyan Liu,Yanjuan Liu,Yuefei Zhang,Wei Chen,Sheng Tang
In this work, zeolitic imidazolate framework-67 (ZIF-67) with excellent stability synthesized at room temperature was used together with amphiphilic polymer hydrogel to synthesize a captivating mixed-mode silica stationary phase for the first time. The amphiphilic polymer hydrogel prepared by weakly basic cationic and acidic anionic monomers that was modified on the surface of ZIF-67@SiO 2 by a simple physical coating method not only improved the separation performance, but also enhanced the applicability of ZIF-67@SiO 2 in chromatographic analysis. Meanwhile, the porous ZIF-67 effectively alleviated the problem that polymer hydrogel was easy to swell. To sum up, the amphiphilic polymer hydrogel and ZIF-67 showed excellent synergistic effect in improving the separation ability and the applicability of stationary phase. The experimental results demonstrated that the ZIF-67/hydrogel@SiO 2 stationary phase could be applied in various chromatographic separation modes, demonstrating superior resolution and separation selectivity for polycyclic aromatic hydrocarbons, steroid hormones, nucleosides, B-vitamins, sulfonamides, benzoic acids and dinitrobenzene isomers. In this study, the synergistic expression of ZIF-67 and polymer hydrogel provided a new idea for the development of silica stationary phase co-modified by metal-organic framework and hydrogel material. Concurrently, the successful preparation of ZIF-67/hydrogel@SiO 2 composite revealed a new possibility for utilizing ZIF-67 as the functional material of stationary phase, expanding the application potential of ZIF-67 in the field of chromatography.
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MICROCHEMICAL JOURNAL
·
2024
·
IF 4.9
Tong Ren,Zhen Feng,Fang Jiang,Xingtong Liu,Tingting Chen,Yanli Guo,Lei Tian,Xiao-Feng Kang,Fujun Yao
Guanine and its derivatives play fundamental roles in many biological processes and their abnormal changes are closely related to diseases. Thus, accurate and sensitive detection of them is beneficial for the early diagnosis and clinical medicine. Herein, a novel nanopore-based sensor is proposed to detection guanine and its derivatives by using a vacancy G-quadruplex (vG4) probe. In this design, the incomplete G-tetrad in vG4 probe can be filled in by guanine derivatives through Hoogsteen hydrogen bond interactions, resulting in stabilization of the G-quadruplex. Based on the different electronic signals between vG4 probe and its binding complexes, the nanopore sensor was able to achieve the detection of six guanine derivatives, including 2΄-dG, Guanine, Guanosine, GMP, GDP and GTP. To demonstrate the analytical performance of the method, a guanine analogue drug was determined as model analyte. The detection limit of acyclovir was 0.0061 μM (3 σ / k ), with a linear range of 0.01 μM – 0.1 μM. This sensing strategy offers a new pathway for label-free detection of nucleobases and derivatives.
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Journal of Analysis and Testing
·
2025
·
IF 7
Chen Jiajing,Lin Juan,Ouyang Dan,Lin Zian
Metabolomics, based on laser desorption/ionization mass spectrometry (LDI-MS), has been successfully utilized for the high-throughput metabolic analysis of biofluids. This technique shows great promises as a powerful tool for disease screening. Although various nanomaterials have been developed as alternatives to traditional organic matrices in LDI-MS, the signals of most metabolites are limited due to their low abundance in complex biofluids. Herein, four hydroxyl-functionalized covalent organic frameworks (COFs) were designed as substrates for LDI-MS, named COF-OH- n ( n = 0–3, demonstrating the number of hydroxyl units). Since hydroxyl groups can facilitate proton transfer and promote the ionization process effectively, hydroxyl-rich COF-OH-2 enabled sensitive and efficient LDI-MS analysis of serum directly, resulting in highly reproducible serum metabolic profiles (SMPs). An orthogonal partial least squares discriminant analysis (OPLS-DA) model was successfully used to distinguish 30 gout patients from 38 healthy volunteers, with an area under the curve (AUC) of 0.974. Furthermore, the roles of 12 biomarker candidates, which were characterised following statistical analysis, in the metabolic pathway of gout were initially explored. Furthermore, the roles of 12 biomarker candidates, which were characterized following statistical analysis, in the metabolic pathway of gout were initially explored. This work demonstrates the potential of COF-OH-2-assisted LDI-MS in clinical metabolic analysis and offers a rational design strategy for advanced LDI-MS substrates.
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ANALYTICA CHIMICA ACTA
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2015
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IF 4.513
Qing Wang,Mao Ye,Li Xu,Zhi-guo Shi
A mixed-mode chromatographic packing material, C18 and diol groups modified silica (C18-Diol), was prepared with controllable hydrophobicity and hydrophilicity . It demonstrated excellent aqueous compatibility and stability in aqueous mobile phase ; compared to the traditional C18 column, improved peak shape of basic analytes was also obtained. Additionally, it exhibited both reversed-phase liquid chromatographic (RPLC) and hydrophilic interaction chromatographic (HILIC) performance; the analyte separation scope was thus enlarged, demonstrated by simultaneous separation of twenty acids, bases and neutrals. More interestingly, a novel on-line two-dimensional liquid chromatography on the single column (2D-LC-1C) was established by modifying the high performance liquid chromatographic instrument only with the addition of an extra six-port two-position valve. The early co-eluted components of the extract of Lonicera japonica on the 1st-dimension (RPLC) were collected for the online re-injection to the 2nd-dimension (HILIC) by conveniently varying the mobile phase components. Six more peaks were obtained. The established system was simple, easy operation and low cost, which had advantages in analyzing complicated samples.
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ANALYTICAL SCIENCES
·
2018
·Vol. 34
·期 4
·433-438
·
IF 1.355
Li Hengye,Zhang Xuemeng,Zhang Lin,Cang Hui,Kong Fenying,Fan Dahe,Wang Wei
Surface-initiated anionic-ring-opening multibranching polymerization was employed to prepare a hyperbranched polyglycerol (HPG) functionalized silica stationary phase for hydrophilic interaction liquid chromatography (HILIC). The obtained stationary phase was characterized by Fourier-transform infrared spectrometry (FT-IR) and thermogravimetric analysis (TGA). The chromatographic properties of the prepared stationary phase were systematically investigated. The abundance and multitude distribution of hydroxyl groups in HPG endowed the stationary phase with improved hydrophilicity and enhanced separation performance compared with the stationary phase functionalized with monolayer of hydroxyl groups. The stationary phase showed excellent retention of various polar compounds, such as nucleosides, necleobases, phenols and sulfanilamides, indicating great potential in the separation of complex biosamples.
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JOURNAL OF CHROMATOGRAPHY A
·
2016
·
IF 3.926
Hengye Li,Xuemeng Zhang,Lin Zhang,Xiaojin Wang,Fenying Kong,Dahe Fan,Lei Li,Wei Wang
In this study, a boronate affinity silica stationary phase with enhanced binding properties towards cis -diol compounds was prepared through the combination of surface-initiated atom transfer radical polymerization (SI-ATRP) with a Wulff-type boronate as affinity ligand. The stationary phase showed good hydrophilicity and improved binding strength toward adenosine, with binding constant to be as low as 2.38 × 10 −4 M. The column exhibited excellent binding specificity, low binding pH (≥5.5) and high binding capacities (80.1 μmol adenosine g −1 at pH 7.0 and 45.2 μmol adenosine g −1 at pH 5.5, respectively). The stationary phase was applied as adsorbent for the selective extraction of nucleosides in human urine with excellent specificity and high enrichment efficiency. These results demonstrated that this stationary phase could be favorably applied for selective capture and enrichment of cis -diol compounds in complex samples.
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