CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Wen Ma,Mingxia Liu,Mengling Tu,Gang Wang,Jun Li,Fen Liu,Jian Yang,Xianjiang Li
Five two-dimensional multi-layered MXenes namely MO 2 C, Ti 2 C, V 2 C, Nb 2 C and Ta 2 C were synthesized by a one-step exfoliation process and evaluated as laser desorption ionization mass spectrometry (LDI-MS) matrices for fast detection of small biomolecules for the first time. Among them, Nb 2 C exhibited the best performance due to its high carrier mobility, strong photo-induced charge transfer resonance and good UV absorption ability. A simple, universal and efficient LDI-MS platform was established for small biomolecule analysis based on the Nb 2 C matrix. Key factors that affect LDI-MS efficacy were investigated and the established method demonstrated ultraclean MS background, high sensitivity with detection limits low to fmol level and good reproducibility. The Nb 2 C-based LDI-MS platform was successfully applied in the rapid determination of 13 amino acids (AAs) in human serum and 3 AAs, as potential biomarkers, were found to be significantly down-regulated in major depressive disorder patients. This work proved the feasibility of Nb 2 C MXene as an LDI-MS matrix and provided a promising and universal platform for the rapid detection of small molecules in biomedical research.
研究领域:
分析化学
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生物医学
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材料科学
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产品关联
DOI
高影响因子
ANALYTICAL CHEMISTRY
·
2022
·
IF 8.008
Ke Min,Yong Li,Yue Lin,Xuezhi Yang,Zigu Chen,Bo Chen,Ming Ma,Qian Liu,Guibin Jiang
Soot, mainly derived from incomplete combustion of fossil fuel and biomass, exists ubiquitously in different environmental matrixes. To study the detrimental effects of soot on climate, air quality, and human health, accurate quantification of soot is an important prerequisite. However, until now, quantification of soot in environmental media, especially in carbonaceous media, is still very challenging. Here, we report a matrix-free laser desorption/ionization mass spectrometry (LDI-MS) method for in situ imaging of soot particles in size-segregated aerosol samples collected on filter membranes. A series of round-shaped sample spots in filter membranes were selected and subjected to MS imaging analysis, enabling direct in situ quantification of soot without solvent extraction or separation. Especially, the MS imaging with serial sample spots can overcome the problems of sweet-spot in LDI-MS and inhomogeneous distribution of soot in the filter membrane, thus greatly improving the precision of quantification. The limit of detection of soot was 4 ng/m2 and the recovery was 84.4–126%. By using this method, we found that a higher soot content was present in larger-sized particulate matter than smaller-sized particles, suggesting that aerosol soot was mainly derived from primary emission sources. Furthermore, this method also shows the potential to analyze nitrate and sulfate species in PM2.5. To the best of our knowledge, it is the first method capable of simultaneous analysis of inorganic salts and soot in air samples. It represents a novel strategy for in situ quantification of aerosol soot with the advantages of high specificity, high sensitivity, separation-, solvent- and matrix-free.
研究领域:
环境科学
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分析化学
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产品关联
DOI
PubMed
高影响因子
MICROCHIMICA ACTA
·
2021
·Vol. 188
·期 1
·1-11
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IF 5.833
Lv Yuanxia,Qin Xiaohuan,Hu Kun,Huang Yong,Zhao Shulin
A novel matrix-assisted laser desorption/ionization time-of-flight mass spectrometric method (MALDI-TOF MS) for determination of highly sensitive small molecular compounds was developed based on molybdenum disulfide nanosheets hybridized with ultrathin graphitic carbon nitride (MoS 2 /g-C 3 N 4 ) as the matrix. With this approach, the synergistic effects of MoS 2 and g-C 3 N 4 enhance the UV absorption of MoS 2 /g-C 3 N 4 , increase both desorption and ionization efficiency in LDI MS, and induce higher signal-to-noise ratio of analytes when compared with the bare MoS 2 and g-C 3 N 4 matrix in the determination of amino acids, antibiotics, neutral oligosaccharides, uric acid, and polyethylene glycols (PEGs). The detection limits of these small molecular compounds are in the ranges 0.1 to 10 μg mL −1 , 1*10 −3 to 1.0 μg mL −1 , 1.0 to 10 μg mL −1 , and 2*10 −4 μg mL −1 , respectively, and the polydispersity index of these PEGs is less than 1.02. Moreover, high salt tolera`nce and homogeneous deposition on the spot results in good reproducibility. The relative standard deviations (RSDs) of shot-to-shot and spot-to-spot ( n = 15) of these compounds are less than 10.1% and 12.5%, respectively. With MoS 2 /g-C 3 N 4 , the uric acid in complicated biological samples can be directly determined in combination with LDI-TOF MS. Graphical abstract
We synthesized MoS 2 /g-C 3 N 4 nanohybrid as an efficient matrix for MALDI-TOF MS analysis of small molecules as well as quantitative detection of uric acid in human urine.
研究领域:
分析化学
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生物医学
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DOI
高影响因子
ACS Omega
·
2019
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IF 2.584
Shumei Yang,Lei Mu,Ruxia Feng,Xianglei Kong
Matrix-assisted laser desorption/ionization mass spectrometry (MALDI MS) has shown its great success in the qualitative analysis of a wide range of organic and biological molecules. However, its application in quantitative analysis is still limited by the difficulty in the availability of isotope-labeled internal standards. The present work investigates the relationship between the correlation coefficient of the peak intensities of analyte and candidate internal standard ions and the linearity of possible quantitative analysis. Based on the two analyte examples, ciprofloxacin and substance P, the results show that the performance of the selected nonisotope-labeled internal standard is greatly related to the correlation coefficient. A high positive correlation coefficient (>0.7) between the ions of analyte and candidate standard can result in a good linearity (R2 > 0.98) and vice versa. The results provide a new way to select nonisotope-labeled internal standards for MALDI analysis and thus can be potentially applied in the rapid quantitative mass spectrometry.
研究领域:
分析化学
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生物医学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Yanfang Zhao,Rabah Boukherroub,Lu Liu,Huizhi Li,Ru-Song Zhao,Qin Wei,Xiang Yu,Xiangfeng Chen
Bisphenol A (BPA) displays harmful effects on the human health, including potent endocrine activity and potential impact on the development of cancer. Analysis BPA residues in water and plastic products attracted considerable attention in the past decades. However, dominantly used conventional analysis techniques are unable to directly and non-destructively identify the correct species of BPA in plastic products. Hence, this study demonstrates the effective utilisation of boron nitride quantum dots (BNQDs) as an inorganic matrix in matrix-assisted laser desorption/ionization mass spectrometry analysis and imaging (MALDI-MS & MSI) for BPA. The presence of abundant hydroxyl and amino groups on the BNQDs’ surface is favourable for the formation of hydrogen bonds with BPA, and increases their ionization and chemoselectivity. Intriguingly, the BNQDs matrix offers a distinct signal for phenolic hazardous molecules featuring different hydroxyl groups. The method was applied to detect BPA at nanomolar level in environmental water, and also allowed non-destructive and in situ mapping of BPA in plastics and pacifiers. This research provides a novel strategy for adapting nanomaterials as inorganic matrices for analysis of small molecular pollutants in environmentally relevant samples using MALDI-MS & MSI.
研究领域:
分析化学
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环境科学
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毒理学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF PHARMACEUTICAL AND BIOMEDICAL ANALYSIS
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2019
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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
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分子生物学
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癌症研究
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代谢组学
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DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2018
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IF 8.097
Xiaoming Chen,Tao Wang,Leimiao Lin,Fangjie Wo,Yaqin Liu,Xiao Liang,Hui Ye,Jianmin Wu
Nanostructured semiconductors are one of the most potent candidates for matrix-free laser desorption/ionization mass spectrometric (LDI-MS) analysis of low-molecular-weight molecules. Herein, the enhanced photoinduced electron transfer and LDI on the tip of a vertical silicon nanowire (SiNW) array were investigated. Theoretical simulation and LDI detection of indigo and isatin molecules in negative ion mode revealed that the electric field can be enhanced on the tip end of SiNWs, thereby promoting the energy and electron transfer to the analytes adsorbed on the tip of SiNWs. On the basis of this finding, a tip-contact sampling method coupled with LDI-MS detection was established. In this strategy, the tip of SiNWs can be regarded as microextraction heads for the sampling of molecules when they come in contact with analytes. Impression of skin, tissue, and pericarp on the vertical SiNW array can effectively transfer endogenous metabolites or exogenous substances onto the tip. Upon laser irradiation, the adsorbed molecules on the SiNW tip can be efficiently ionized and detected in negative ion mode because of the tip-enhanced electron transfer and LDI effect. We believe this work may significantly expand the application of LDI-MS in various fields.
研究领域:
分析化学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL PHYSICS LETTERS
·
2023
·
IF 2.8
Huaqing Lin,Ming Yin,Chenjie Yang,Dongpo Xu,Chunhui Deng
Laser desorption/ionisation mass spectrometry (LDI-MS) can be used as an effective detection method for the analysis of more complex samples. However, the organic matrix of conventional LDI-MS produces large background interference and poor signal results, which hinders its application in metabolomics. Surface reconstruction can improve the performance of LDI-MS. In this study, mesoporous NiO@Pt nanofibre membranes were synthesised by a simple and efficient electrostatic spinning strategy and used as a matrix to significantly increase the intensity of mass spectrometry peaks. Metabolomic analysis of saliva samples from 18 smokers and 15 non-smokers was able to clearly distinguish the differences in salivary metabolism between smokers and non-smokers and showed good results in the qualitative analysis of salivary metabolism in smokers. Our study provides a rapid and convenient method for differentiating differences in salivary metabolism in smokers.
研究领域:
分析化学
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代谢组学
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医学诊断
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产品关联
DOI
高影响因子
ANALYTICAL CHEMISTRY
·
2022
·
IF 8.008
Liuying He,Xiao Wang,Junyu Chen,Yuze Li,Liping Wang,Caiqiao Xiong,Zongxiu Nie
Liver cancer (LC) is the third frequent cause of death worldwide, so early diagnosis of liver cancer patients is crucial for disease management. Herein, we applied NH2-coated polystyrene@Fe3O4 magnetic beads (PS@Fe3O4–NH2 MBs) as a matrix material in laser desorption/ionization mass spectrometry (LDI-MS). Rapid, sensitive, and selective metabolic profiling of the native biofluids was achieved without any inconvenient enrichment or purification. Then, based on the selected m/z features, LC patients were discriminated from healthy controls (HCs) by machine learning, with the high area under the curve (AUC) values for urine and serum assessments (0.962 and 0.935). Moreover, initial-diagnosed and subsequent-visited LC patients were also differentiated, which indicates potential applications of this method in early diagnosis. Furthermore, among these identified compounds by FT-ICR MS, the expression level of some metabolites changed from HCs to LCs, including 29 and 12 characteristic metabolites in human urine and serum samples, respectively. These results suggest that PS@Fe3O4–NH2 MBs-assisted LDI-MS coupled with machine learning is feasible for LC clinical diagnosis.
研究领域:
医学
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分析化学
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肿瘤学
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产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry B
·
2020
·Vol. 8
·期 34
·7792-7800
·
IF 5.344
Rui Lv,Enhui Wu,Renfei Wu,Wen Shen,Chongqing Ma,Rui Shi,Ruochen Guo,Mingwang Shao,Jian Liu
There is increasing demand for anti-doping drug monitoring in sports and food safety checks by developing sensitive and fast analytical methods. Here we report the development of hybrid Ir/SiNW as a new MALDI matrix for the detection of small molecules. This matrix is characterized by sufficient UV absorption, low-noise background, and high efficiency in ionization of small molecules. Sensitive detection of clenbuterol (LOD: 0.18 pmol) and a variety of other small molecules has been achieved using the Ir/SiNW matrix with a reproducible performance. Compared to the individual components separately, the matrix of hybrid Ir/SiNW synthesized via in situ growth can promote the MS signal intensity by up to 10 fold under identical experimental conditions. We provide a unique mechanism for the high performance of the hybrid Ir/SiNW matrix with the characteristic properties of hydrogen atom transfer and enhanced protonation at the interface of the hybrid nanostructures. Our approach of using a hybrid Ir/SiNW matrix enables detection of clenbuterol quantitatively in complicated biological samples and in vivo experiments, promising a useful tool for food security and anti-doping drug monitoring in sports.
研究领域:
分析化学
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食品科学
·
运动医学
✓ 已验证
DOI
PubMed
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
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分析化学
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产品关联
DOI
高影响因子
ANALYST
·
2020
·Vol. 145
·期 8
·3125-3130
·
IF 3.978
Dan Ouyang,Kailong Luo,Wende Ma,Jie Wu,Jing Li,Yanting He,Zongwei Cai,Zian Lin
A spherical vinyl-functionalized covalent-organic framework (COF-V) was prepared at room temperature by a facile method and applied as a novel substrate for surface-enhanced laser desorption/ionization mass spectrometry (SELDI-MS). Compared with conventional organic matrices, the spherical COF-V with high crystallinity and good monodispersity exhibited high sensitivity, no matrix background interference, wide-range applicability, high salt tolerance and reproducibility in the characterization of small molecules. Considering these advantages, the applicability of the spherical COF-V-based SELDI-MS method was successfully demonstrated by determining trace amounts of glucose in diabetic urine, which would be a promising candidate for clinical diagnosis of diabetes. In addition, the morphological effect and the desorption/ionization mechanism of the COF-V were investigated in detail and the results indicated that the spherical COF-V substrate could greatly enhance the LDI process compared with the bulk COF-V. This work not only extends the application of COFs in MS, but also offers a promising alternative for small molecule identification and clinical diagnosis of diabetes.
研究领域:
分析化学
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医学诊断
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）