Analytical Methods
·
2019
·Vol. 11
·期 8
·1131-1136
·
IF 2.378
Yueying Zhang,Dan Gao,Shangfu Li,Weili Wei,Jinshun Lin,Yuyang Jiang
1,5-Diaminonaphthalene functionalized carbon nanodots (DAN-CDs) were explored as a novel matrix for direct detection of small molecules by matrix-assisted laser desorption/ionization mass spectrometry (MALDI-MS) in negative ion mode. By using DAN-CDs as the matrix, we could detect not only biological small molecules such as fatty acids (FAs), amino acids, peptide Gly–Gly and dopamine, but also anticancer drug erlotinib. By comparison with the performance of CDs, DAN, and their binary matrix, DAN-CDs were favored because of their lower matrix background interference and good detection sensitivity. In addition, the DAN-CDs matrix displayed good salt tolerance and was further applied for plasma detection and qualitative detection of endogenous FAs in a plasma sample. Furthermore, the covalent amide bonds in the DAN-CDs matrix reduced signal interference from the matrix. These results demonstrated that DAN-CDs are a novel negative ion mode matrix for the analysis of small molecules in bio-samples by MALDI-MS.
研究领域:
分析化学
·
生物医学
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DOI
高影响因子
ANALYTICAL BIOCHEMISTRY
·
2020
·
IF 2.877
Zhijing Song,Huanyu Gao,Wenchun Xie,Qing Sun,Kai Liang,Yan Li
Measuring the concentrations of steroid hormones in plasma is critical for understanding their role in various vital physiological processes . The detection of underivatized steroid hormones in biofluids through mass spectrometry (MS) is typically hindered by low ionization efficiency. We described a novel matrix-assisted laser desorption/ionization-MS (MALDI-MS) approach based on hydroxylamine derivatization (HA-D) to analyze low-concentration steroid hormones in plasma. The ketonic carbonyl group containing steroid hormones could be derivatized using HA to form oxime derivatives, which considerably enhanced the MS sensitivity for detecting steroid hormones. By using the optimized conditions, estrone (E1), testosterone (T), and progesterone (Prog), could be simultaneously quantified in plasma with a limit of detection (LOD) from 0.019 to 0.031 nM, recoveries from 86% to 108%, and coefficient of variation (CV%) from 4.59% to 11.90%. HA-D/MALDI-MS exhibited higher sensitivity than those using Girard T (GT). To establish potential utility of our method, we characterized fatty liver patient plasmas to demonstrate that the HA-D/MALDI-MS procedure could generate quantitative results comparable to the current clinical liquid chromatography-electrospray ionization tandem MS (LC-ESI MS/MS) method. This approach facilitates the rapid and accurate characterization of plasma hormones , and renders the MALDI-MS approach for steroid hormones more adaptable for clinical research and use.
研究领域:
生物化学
·
医学检验
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DOI
PubMed
高影响因子
JOURNAL OF PHARMACEUTICAL AND BIOMEDICAL ANALYSIS
·
2019
·
IF 2.983
Chenglong Sun,Zhichao Li,Chunxia Ma,Qingce Zang,Jiangshuo Li,Wei Liu,Hengqiang Zhao,Xiao Wang
Profiling the endogenous tissue metabolites with spatial features is significant for our understanding of molecular histology, and provides an insightful way to uncover the complex associations between tissue metabolic response and external stimuli. Matrix-assisted laser desorption/ionization mass spectrometry imaging (MALDI-MSI) is an effective molecular imaging technology to illustrate the spatial locations of molecules in tissue. However, due to the limited sensitivity and the presence of multiple matrix-related ions, it is still challenging to globally image the small molecule metabolites (SMMs) using MALDI, especially for those low-content functional ones. Here, a simple acetone washing method was developed to improve the sensitivity of MALDI-MS for imaging SMMs. After immersing in acetone and shaken for 15 min, key functional SMMs were well-visualized with significantly enhanced ion intensities. In addition to lipids, more than 160 SMM ions, including polyamines, cholines, carnitines, amino acids, nitrogenous bases, nucleosides, carbohydrates, organic acids, vitamins were imaged. The acetone washes-based MALDI-MSI was then applied to profile the metabolic alternations that occurred in osteosarcoma, and the abnormally altered SMMs and lipids were clearly visualized. Moreover, with the protection of acetone against tissue antigenicity, we successfully characterized the expression of three metabolites-related enzymes, fatty acid synthase (FASN), glutaminase (GLS), and cytosolic phospholipase A2 (cPLA2) in osteosarcoma. The spatially-resolved metabolite and corresponding enzyme information reveals what occured in osteosarcoma at the molecular level, providing new insights into the understanding of tumour metabolic reprogramming.
研究领域:
分析化学
·
分子生物学
·
癌症研究
·
代谢组学
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DOI
PubMed
高影响因子
RSC Advances
·
2018
·Vol. 8
·期 46
·26116-26123
·
IF 2.936
Ran Wang,Yufei Liu,Chang Wang,Henghui Li,Xin Liu,Liming Cheng,Yanhong Zhou
Monitoring serum glycomics is one of the most important emerging approaches for diagnosis of various cancers, and the majority of previous studies were based on MALDI-MS or HPLC analysis. Considering the difference of these analytical methods employed for serum glycomics, it is necessary to compare the effectiveness of different analytical methods for monitoring the aberrant changes in serum glycomics. In this study, a strategy based on machine learning was firstly applied for comparing the analysis results of MALDI-MS and HPLC on the same serum glycomics of hepatocellular carcinoma (HCC) samples. The capability of these two analytical methods for identifying HCC is demonstrated by the classification results obtained from MALDI-MS and HPLC data. In addition, by comparing glycomics which were significantly correlated with HCC based on MALDI-MS and HPLC, some N-glycans which may be the potential biomarkers for HCC were identified, validating the capability of these two analytical methods for the differentiated identification in the analysis of glycomics. Meanwhile, it is noteworthy that various physiological and environmental factors may cause the aberrant changes in glycosylation, and all these interference factors may be minimized by analyzing the same sample sets of HCC. Overall, these results showed that MALDI-MS and HPLC are complementary in qualitative and quantitative analysis of serum glycomics.
研究领域:
生物化学
·
癌症研究
·
分析化学
·
机器学习
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DOI
PubMed
高影响因子
PLoS One
·
2017
·Vol. 12
·期 1
·e0170013
·
IF 2.806
Sheng Liu,Wenjie Gao,Yao Wang,Zhenyu He,Xiaojun Feng,Bi-Feng Liu,Xin Liu
Monitoring glycosylation of the mAbs have been emphasized and routinely characterized in biopharmaceutical industries because the carbohydrate components are closely related to the safety, efficacy, and consistency of the antibodies. In this study, the comprehensive glycan profiling of a biosimilar candidate of cetuximab was successfully characterized using Normal phase high-performance liquid chromatography (NP-HPLC) in combination with Matrix assisted laser desorption/ionization mass spectrometry (MALDI-MS). The presence of minor N-linked glycans containing sialic acid lactone residues (NeuAcLac) was observed in the biosimilar for the first time, which could influence the quantitative analysis of sialylated glycans and interfere with quantification of neutral glycans when it was analyzed by high performance liquid chromatography fluorescence (HPLC-FL). To overcome this issue, mild alkali treatment was used to hydrolyze lactone of the sialic acid to their neutral formation, which had no impact on the analysis of other glycans before and after the treatment. As a result, the mild alkali treatment might be helpful to obtain quantitative glycan profiling of the mAbs drugs with enhanced accuracy and robustness.
研究领域:
生物制药
·
蛋白质组学
·
药物分析
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DOI
PubMed
高影响因子
Journal of Analysis and Testing
·
2022
·Vol. 6
·期 4
·419-423
·
IF 0
Tong Yi,Liu Zheng-Zheng,Lu Jia-Feng,Zhang Hai-Yan,Shi Ke-Qiang,Chen Guan-Ru,Liu Ya-Qin,Feng Hong-Ru,Pan Yuan-Jiang
Halogens are elements in soil and water that occur as organic and inorganic species. Studies have shown that inorganic halogens are closely related to animal and plant life. Matrix-assisted laser desorption/ionization mass spectrometry (MALDI-MS) can achieve high-throughput and rapid analysis, which is also an essential characteristic in some environmental studies. However, there is currently no report on MALDI-MS analysis for water-soluble inorganic halogen compounds. In this study, we aimed to develop a reliable and reproductive method to detect inorganic halogens in soil and water by MALDI-MS. Based on sinapic acid (SA) and silver trifluoromethanesulfonate (SA/AgOTf) as the matrix in negative-ion mode, MALDI-MS showed excellent MS signals related to halogens. Under the optimum conditions, the method achieved satisfactory linearity ( R 2 > 0.99) and repeatability (RSD < 18%). The LODs for Cl − , Br − and I − were 0.76, 0.11 and 0.10 μg/mL, respectively. The concentration of inorganic halogens from 24 samples was successfully determined by MALDI-MS. In summary, an innovative method was developed for the analysis of inorganic halogens by MALDI-MS using a novel SA/AgOTf matrix, extending the application of MALDI-MS in inorganic compounds.
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TALANTA
·
2020
·
IF 5.339
Ning Li,Shuzhen Dou,Lei Feng,Qunyan Zhu,Nan Lu
In matrix-assisted laser desorption/ionization mass spectrometry (MALDI-MS), the analyte is usually distributed unevenly throughout the sample spot. The area with aggregated analyte molecules contributing abundant signal, is termed as “sweet spot”, which results in poor detection reproducibility and makes it impossible to quantify analytes without internal standards. We proposed a strategy to eliminate sweet spot in MALDI-MS by using a hydrophobic ordered structure as target. The target is fabricated by creating a hydrophobic silicon nanopillar array and subsequently decorating it uniformly with poly(methyl methacrylate) nanodots for capturing analytes. The sweet spot is eliminated by distributing analyte molecules uniformly on this target, and then result in a uniform MS image, which demonstrates an ideal reproducibility. Finally, with the target assisted MALDI-MS as biosensor was suitable to analyze practical sample such as bacitracin A in milk. Horse heart myoglobin and, angiotensin III molecules can be quantified without internal standard using α-cyano-4-hydroxycinnamic acid as matrix. This biosensor presented good linearity, high salts tolerance and high signal-to-noise ratio (up to 271.8), even the 1 mol/L salt concentration. This strategy could provide an alternative for improving the performance of MALDI-MS.
研究领域:
分析化学
·
生物医学工程
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DOI
PubMed
高影响因子
ANALYTICA CHIMICA ACTA
·
2016
·
IF 4.712
Henghui Li,Wenjie Gao,Xiaojun Feng,Bi-Feng Liu,Xin Liu
Sialic acids usually locate at the terminal of many glycan structures in either α(2,3) or α(2,6) linkage, playing different roles in various biological and pathological processes. Several linkage specific carboxyl derivatization methods have been reported to discriminate between α(2,3) and α(2,6)-linked sialic acids by matrix-assisted laser desorption/ionization mass spectrometry (MALDI-MS). Among them, ethyl esterification was recently reported to achieve linkage specific derivatization between α(2,3) and α(2,6)-linked sialic acids with good selectivity . However, the method suffered from the instability of the generated lactones and byproducts of the derivatives. To overcome these shortcomings, a solid-phase two step derivatization method was introduced to convert the α(2,6)-linked sialic acid into ethyl esters and the α(2,3)-inked counterparts into N-methyl amides, respectively. Under the optimized derivatization conditions, our method was able to achieve accurate relative quantification of N-glycan as well as their corresponding sialylated linkage types, superior to the ethyl esterification method. The solid phase derivatization strategy was further applied to investigate N-glycans from biosimilar antibody drug and human serum from patients and healthy volunteers. This method has the potential to be used in the biomarker discovery and pharmaceutical industry .
研究领域:
分析化学
·
药学
·
生物化学
·
临床化学
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DOI
PubMed
高影响因子
ANALYTICAL CHEMISTRY
·
2026
·
IF 7.3
Lu Xiaochen,Han Jing,Chen Hongwei,Wang Shengjie,Cong Wenkai,Qi Guanghong,Nie Zongxiu
Central nervous system (CNS) infections represent a common
but
serious complication following neurosurgical procedures. However,
the metabolic alterations induced by infection remain incompletely
understood, and noninvasive monitoring strategies remain urgently
needed. In this study, we conducted a systematic metabolomic analysis
of two biofluids─cerebrospinal fluid (CSF) and urine─obtained
from patients undergoing neurosurgical procedures, using matrix-assisted
laser desorption/ionization mass spectrometry (MALDI-MS). Metabolomic
analysis of CSF revealed significant metabolic reprogramming associated
with CNS infections, primarily characterized by the dysregulation
of energy metabolism, amino acid metabolism, lipid and membrane-related
pathways. Interestingly, similar pathway perturbations were also observed
in the urinary metabolome. We further observed a significant comprehensive
correlation between the urinary and CSF metabolomes. Then, machine
learning models were successfully constructed based on urinary metabolomic
features for noninvasive disease diagnosis and prognostic evaluation.
Both the diagnostic and prognostic models achieved satisfactory classification
performance, with area under the receiver operating characteristic
curve values greater than 0.9. This work presents a novel, rapid,
and noninvasive strategy for the detection and clinical management
of CNS infections, which may facilitate timely and accurate clinical
intervention and ultimately improve patient outcomes.
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高影响因子
TALANTA
·
2018
·
IF 4.244
Xueyun Wang,Ning Li,Daren Xu,Xiangchao Yang,Qunyan Zhu,Dongyang Xiao,Nan Lu
Superhydrophobic substrate is applied in matrix-assisted laser desorption/ionization mass spectrometry (MALDI MS) detection due to its confinement effect. The weak interaction of superhydrophobic surface with water/salts makes it potential in one-step enrichment and desalting of peptide in MALDI MS analysis. We fabricate a superhydrophobic substrate by spin-coating poly(dimethyl siloxane) (PDMS) on a candle soot layer. On this substrate, the peptide analytes can be confined and enriched in a small area due to the confinement effect and its strong hydrophobic interactions with PDMS. Meanwhile, the desalting can be easily realized by removing the residual solution after the absorption of analyst molecules due to the weak interaction between water/salt contaminants and the superhydrophobic surface. Using this substrate, angiotensin III (Ang III) in the presence of salt with high concentration (2 M or saturated) can be analyzed, and the peptide sequence coverage of 10 μg/mL myoglobin (MYO) and bovine serum albumin (BSA) digests is enhanced to 51% and 26%, which is 37% and 21% analyzed with the commercial ZipTipC 18 pipette tips. The LOD of bacitracin A (Bac A) in milk with this substrate is 100 pM and nearly 360 times lower than the LOD of standard testing method. This substrate has potential practical applications in proteomics research and actual sample analysis.
研究领域:
分析化学
·
蛋白质组学
·
生物医学
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DOI
高影响因子
INTERNATIONAL JOURNAL OF MASS SPECTROMETRY
·
2020
·
IF 2.09
Xing-Li Pei,Xiao-Ning Liu,Jia-Lin Du,Can Gong,Xu Xu
Matrix application is a critical step in matrix-assisted laser desorption/ionisation mass spectrometry imaging (MALDI-MSI) analysis. Here, we describe a low cost, small size, and portable ultrasonic spraying device for various matrix deposition that is ideal for applying to obtain micron-sized (about 1–15 μm) cocrystallisation . The ultrasonic spray method was systematically compared with mainstream matrix application approaches based on optimization experiments. In the approach, ethanol was used as the solvent, and the spray direction was perpendicular to the MALDI sample slide. Seven different matrices were compared and we found that 2-[(2E)-3-(4- tert -butylphenyl)-2-methylprop-2-enylidene] malononitrile (DCTB) is a more suitable matrix for the detection of triacylglycerol (TAGs) and phosphatidylcholines (PCs) than other matrices. The DCTB matrix solution with concentrations of 5 mg mL −1 was applied on the surfaces of corn sections through ultrasonic spraying. The corn sections were then analysed through MALDI-MS in positive ion mode. MALDI-MSI allowed the simultaneous detection of multiple lipids including 16 TAGs and PCs in corn. The results demonstrated that the ultrasonic spraying device enables the deposition of MALDI matrix solution and provides the advantages of homogeneous micron-sized matrix crystallisation and satisfactory reproducibility.
研究领域:
植物学
·
分析化学
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DOI
高影响因子
TALANTA
·
2020
·
IF 5.339
Yifang Zhang,Zhaoyu Hu,Chun Zhang,Bi-Feng Liu,Xin Liu
Chemical derivatization of glycans is a common strategy to increase the analytical performance of MALDI-MS-based glycan profiling techniques. Hydrazide , one of the most popular tags, offers important advantages including allowing purification-free procedures. Several hydrazides have thus been used for glycomics combined with an on-target strategy to further simplify the analytical procedures. Usually, gentle heating and mildly acidic conditions with somewhat long reaction times are needed for these hydrazide derivatizations to reach a high reaction efficiency, which makes the current hydrazide tags not yet perfectly conducive to high-throughput analysis. To further optimize these hydrazide tags for high-throughput analysis, based on the structure of a reported hydrazide and the theoretical calculations, a new cationic hydrazide tag, 4-(hydrazinecarbonyl)- N , N , N -trimethylbenzenaminium (HTMBA), was designed, synthesized and tested in this work. HTMBA could completely derivatize glycans at room temperature in several seconds under very mildly acidic conditions (<3% acetic acid). A 19-fold enhancement in the signal intensity was obtained without interference from alkali adduct ions in the MALDI-MS detection of HTMBA-labeled maltoheptaose . To broaden the applicability of HTMBA, an HTMBA on-target derivatization (HOD) strategy was developed and fully validated with maltoheptaose and RNase B, and the method showed a good repeatability and stability. Finally, the HOD strategy was successfully applied to serum samples, 44 glycans in human serum were detected, and the O-acetylation information of sialic acid in horse serum was preserved. These results showed that the HOD strategy was suitable for the MS-based rapid analysis of all glycoforms in complex biological samples.
研究领域:
生物化学
·
分析化学
·
医学
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DOI
PubMed
高影响因子
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