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MALDI coupled with laser-postionization and trapped ion mobility spectrometry contribute to the enhanced detection of lipids in cancer cell spheroids

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Chinese Chemical Letters 2024年第4期35卷 464-468页

作者： Jing Chen peisi xie Pengfei Wu Yu He Zian Lin Zongwei Cai Ministry of Education Key Laboratory of Analytical Science for Food Safety and Biology Fujian Provincial Key Laboratory of Analysis and Detection Technology for Food SafetyCollege of ChemistryFuzhou UniversityFuzhou 350116China Department of Chemistry State Key Laboratory of Environmental and Biological AnalysisHong Kong Baptist UniversityHong KongChina College of Forestry Nanjing Forestry UniversityNanjing 210018China

Cancer cell spheroids(CCS) are a valuable three-dimensional cell model in cancer studies because they could replicate numerous characteristics of solid tumors. Increasing researches have used matrix-assisted laser desorption/ionization mass spectrometry imaging(MALDI-MSI) to investigate the spatial distribution of endogenous compounds(e.g., lipids) in CCS. However, only limited lipid species can be detected owing to a low ion yield by using MALDI. Besides, it is still challenging to fully characterize the structural diversity of lipids due to the existence of isomeric/isobaric species. Here, we carried out the initial application of MALDI coupled with laser-postionization(MALDI-2) and trapped ion mobility spectrometry(TIMS) imaging in HCT116 colon CCS to address these challenges. We demonstrated that MALDI-2 is capable of detecting more number and classes of lipids in HCT116 colon CCS with higher signal intensities than MALDI. TIMS could successfully separate numerous isobaric/isomeric species of lipids in CCS. Interestingly, we found that some isomeric/isobaric species have totally different spatial distributions in colon CCS. Further MS/MS imaging analysis was employed to determine the compositions of fatty acid chains for isomeric species by examining disparities in signal intensities and spatial distributions of product ions. This work stresses the robust ability of TIMS and MALDI-2 imaging in analyzing endogenous lipids in CCS, which could potentially become powerful tools for future cancer studies.

关键词： Matrix-assisted laser desorption/ionization(MALDI) Mass spectrometry imaging MALDI coupled with laser-postionization Trapped ion mobility spectrometry Cancer cell spheroids

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Multicellular tumor spheroids bridge the gap between two-dimensional cancer cells and solid tumors: The role of lipid metabolism and distribution

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Chinese Chemical Letters 2023年第2期34卷 259-262页

作者： peisi xie Jinghui Zhang Pengfei Wu Yongjiang Wu Yanjun Hong Jianing Wang Zongwei Cai State Key Laboratory of Environmental and Biological Analysis Department of ChemistryHong Kong Baptist UniversityHong KongChina College of Pharmaceutical Sciences Zhejiang UniversityHangzhou 310058China School of Pharmaceutical Sciences(Shenzhen) Sun Yat-sen UniversityShenzhen 518107China

Previous studies demonstrated that three-dimensional(3D) multicellular tumor spheroids(MCTS) could more closely mimic solid tumors than two-dimensional(2D) cancer cells in terms of the spatial structure, extracellular matrix-cell interaction, and gene expression pattern. However, no study has been reported on the differences in lipid metabolism and distribution among 2D cancer cells, MCTS, and solid tumors. Here, we used Hep G2 liver cancer cell lines to establish these three cancer models. The variations of lipid profiles and spatial distribution among them were explored by using mass spectrometry-based lipidomics and matrix-assisted laser desorption/ionization mass spectrometry imaging(MSI). The results revealed that MCTS, relative to 2D cells, had more shared lipid species with solid tumors. Furthermore,MCTS contained more comparable characteristics than 2D cells to solid tumors with respect to the relative abundance of most lipid classes and mass spectra patterns. MSI data showed that 46 of 71 lipids had similar spatial distribution between solid tumors and MCTS, while lipids in 2D cells had no specific spatial distribution. Interestingly, most of detected lipid species in sphingolipids and glycerolipids preferred locating in the necrotic region to the proliferative region of solid tumors and MCTS. Taken together, our study provides the evidence of lipid metabolism and distribution demonstrating that MCTS are a more suitable in vitro model to mimic solid tumors, which may offer insights into tumor metabolism and microenvironment.

关键词： Lipid metabolism Lipid distribution Two-dimensional cells Three-dimensional cell spheroids Solid tumors

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Identification of glycerophospholipid fatty acid remodeling by using mass spectrometry imaging in bisphenol S induced mouse liver

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Chinese Chemical Letters 2018年第8期29卷 1281-1283页

作者： Chao Zhao peisi xie Ti Yang Hailin Wang Arthur Chi Kong Chung Zongwei Cai State Key Laboratory of Environmental and Biological Analysis Department of Chemistry Hong Kong Baptist University State Key Laboratory of Environmental Chemistry and Ecotoxicology Research Center for Eco-Environmental Sciences Chinese Academy of Sciences

Bisphenol A（BPA） plays an important role in metabolic disorders. As a major alternative to BPA, it is unclear whether the exposure of bisphenol S（BPS） may result in lipidome disturbance. Using a mouse model, we investigated the effects of BPS exposure on metabolism and spatial distribution of lipids by using lipidomics analysis and matrix-assisted laser desorption/ionization（MALDI）-mass spectrometry imaging（MSI） in mouse liver tissues. Lipid metabolites displayed significant up-regulation in phosphatidylethanolamines（PE）, lysophosphatidylcholines（LPC）, lysophosphatidylethanolamines（LPE） and lysophosphatidylserine（LPS） as well as remarkable down-regulation in phosphatidylcholine（PC） and phosphatidylserine（PS） in mouse liver after the exposure at 100 m g BPS/kg body weight/*** obtained results indicated that the lipidome of liver was perturbed significantly in glycerophospholipid（GP） fatty acid remodeling pathway upon the BPS exposure. We applied MSI and multivariate statistical analysis to evaluate the abundance variation of lipid markers in BPS-treated liver sections and to compare with the analytical results from olive oil-treated liver sections. Differential structural lipids with up-regulated PE（20：1/20：4）, LPC（20：4）, LPE（20：4）, LPS（33：4） and down-regulated PC（20：4/22：6）and PS（18：0/22：6）, which were related to GP fatty acid remodeling, changed and co-localized in the liver sections. To explore the cause of variation of lipid abundance, expression of enzymes that regulate biosynthesis and metabolism of fatty acid in liver tissues were analyzed. Consistent with the results of liver lipidome and spatial distribution, a decrease in hepatic expression of LPC acyltransferase 1（LPCAT1）,LPCAT2 and LPS acyltransferase and an increase expression of LPCAT3, LPCAT4, LPE acyltransferase 1（LPEAT1）, LPEAT2 and phospholipase A2 s were observed in GP fatty acid remodeling pathway. Our results demonstrated that exposure to BPS could induce the GP fatty acid remodeling, which m

关键词： Lipidomics MALDI-MSI Bisphenol S Bisphenol A Mouse liver

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Multiple imaging mass spectrometry analyses reveal the evolution of tumor metabolic heterogeneity

Multiple imaging mass spectrometry analyses reveal the evolu...

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2018年中国质谱学术大会（CMSC2018）

作者： Chao Zhao peisi xie Ting Yong Lin Zhu Hailin Wang Zongwei Cai State Key Laboratory of Environmental and Biological Analysis Department of ChemistryHong Kong Baptist University State Key Laboratory of Environmental Chemistry and Ecotoxicology Research Center for Eco-Environmental SciencesChinese Academy of Sciences

We investigated the bisphenol A(BPS)-induced tumor proliferation and deterioration, and potential molecular mechanisms via molecular biology and mass spectrometry(MS)-based lipidomics, proteomics and matrixassisted laser desorption/ionization-MS imaging(MALDI-MSI) in human breast cancer xenograft model. BPS significantly induced proliferation of breast tumor by increased central necrotic domains, accelerated deterioration of breast tumor through enhanced peripheral neoplastic domains. At the molecular level of breast tumor, BPS exposure induced the spatially intratumor heterogeneity of morphology-driven lipids and proteins. Three of proteins associated with chromosomal stability and cell proliferation, the up-regulated ceramides(Cer) and sphingomyelins(SM), and the down-regulated phosphatidylglycerol(PG) were located in central necrotic domains of breast tumor, nine of proteins associated with the stability of nucleic acid structure, as well as un-regulated phosphatidylserine(PS), phosphatidylethanolamine(PE) and phosphatidylinositol(PI) were located in peripheral neoplastic domains. It was suggested that BPS significantly induced tumor proliferation and heterogeneous by the variation of spatial distribution of proteins which were related to chromosomal stability and cell proliferation, as well as the spatial distribution of signaling lipids, reprogramming of DNA methylation and hypoxic tumor microenvironment. Furthermore, our results demonstrated that potential of MS imaging for morphology-driven tumor proliferation, angiogenesis and metastasis induced by environmental pollutants(Fig.1) [1-3].

关键词： Tumor proliferation Lipid metabolism MS Imaging Protein imaging

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两性离子双功能化超亲水金属有机框架纳米复合材料的制备及其用于糖肽的选择性富集

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色谱 2021年第3期39卷 205-210页

作者：李大鹏谢光珊谢佩斯朱林蔡宗苇香港浸会大学环境与生物分析国家重点实验室香港999077

蛋白糖基化是生物体中普遍发生且重要的生物学过程,其参与多种分子生物学的功能和途径,是临床诊断重要的生物标志物。但是,糖肽因其丰度低、离子化效率低、糖链异质性等难点,使糖蛋白分析一直面临巨大的挑战。因此,研究合成了一种新型... 详细信息

蛋白糖基化是生物体中普遍发生且重要的生物学过程,其参与多种分子生物学的功能和途径,是临床诊断重要的生物标志物。但是,糖肽因其丰度低、离子化效率低、糖链异质性等难点,使糖蛋白分析一直面临巨大的挑战。因此,研究合成了一种新型的两性离子双功能化纳米金(AuGC)修饰的超亲水性沸石咪唑骨架(ZIF-8)纳米复合材料(AuGC/ZIF-8),并建立了亲水相互作用色谱(HILIC)和基质辅助激光解吸电离-飞行时间质谱(MALDI-TOF MS)联用选择性富集糖肽的分析方法。谷胱甘肽和半胱氨酸双功能化的协同作用,使MOF具有超亲水性和低空间位阻,为糖肽选择性富集提供了更多的亲和位点。研究以辣根过氧化物酶(HRP)为模式糖蛋白,通过AuGC/ZIF-8富集后,MALDI-TOF MS分析。结果表明,AuGC/ZIF-8对HRP糖肽的富集能力高达250μg/mg,且在与牛血清白蛋白(BSA)混合溶液中(HRP-BSA(1∶200,质量比))显示出对HRP糖肽的高选择性,以及极低含量下(0.3 ng/μL)的高灵敏度。因此,在复杂生物样品糖蛋白的富集分离中具有很大的应用潜力。

关键词：金属有机框架亲水相互作用色谱基质辅助激光解吸电离-飞行时间质谱选择性富集翻译后修饰糖肽

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Airborne fine particulate matter induces cognitive and emotional disorders in offspring mice exposed during pregnancy

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Science Bulletin 2021年第6期66卷 578-591,M0004页

作者： Chao Zhao peisi xie Ting Yong Wei Huang Jianjun Liu Desheng Wu Fenfen Ji Min Li Doudou Zhang Ruijin Li Chuan Dong Juan Ma Zheng Dong Sijin Liu Zongwei Cai State Key Laboratory of Environmental and Biological Analysis Department of ChemistryHong Kong Baptist UniversityHong Kong 999077China Key Laboratory of Modern Toxicology of Shenzhen Shenzhen Center for Disease Control and PreventionShenzhen 518000China School of Chinese Medicine Hong Kong Baptist UniversityHong Kong 999077China Department of Functional Neurology&Neurosurgery First Affiliated Hospital of Shenzhen UniversityShenzhen Second People’s HospitalShenzhen University School of MedicineShenzhen 518000China Institute of Environmental Science Shanxi UniversityTaiyuan 030000China State Key Laboratory of Environmental Chemistry and Ecotoxicology Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China

Gestational exposure to PM_(2.5) is associated with adverse postnatal ***_(2.5) can enter alveoli by using intratracheal instillation,even penetrate through lung cells into the blood ***,they are transferred across the placenta and fetal blood brain barrier,causing the adverse birth outcomes of *** study demonstrated that the gestational exposure resulted in cognitive and emotional disorders in female offspring although the offspring were not exposed to PM_(2.5).Placental metabolic pathways modulated fetal brain development and played a pivotal role for maternal-placentalfetal interactions in the fetal programming of adult behavioral and mental *** of fetus,offspring hippocampus and placenta from the mice exposed to PM_(2.5) were investigated using a comprehensive approach including mass spectrometry-based lipidomics and three-dimensional *** exposure induced the neuro-degeneration in hippocampus,impairment of placental cytoarchitecture,and reprogramming of lipidome,which might affect the modulation of maternal-fetal cross-talk and result in the behavior disorders of *** variation of spatial distribution of lipids was profoundly affected in dorsal pallium and hippocampal formation regions of fetal brain,offspring hippocampus,as well as labyrinth and junctional zones of *** abundance alteration of lipid markers associated with neurodegenerative diseases was validated in transgenic mouse model with Alzheimer’s disease and human cerebrospinal fluid from patients with Parkinson’s *** finding could help with the selection of more suitable heterogeneous-related substructures targeting PM_(2.5) exposure and the exploration of PM_(2.5)-induced toxicological effects on neurodegenerative diseases.

关键词： Airborne fine particulate matter Gestational exposure Lipid metabolism Mass spectrometry imaging Cognitive and emotional disorders

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Multi-layer multi-pass friction rolling additive manufacturing of Al alloy:Toward complex large-scale high-performance components

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International Journal of Minerals,Metallurgy and Materials 2025年第2期32卷 425-438页

作者： Haibin Liu Run Hou Chenghao Wu Ruishan xie Shujun Chen College of Mechanical&Energy Engineering Beijing University of TechnologyBeijing 100124China Chongqing Research Institute of Beijing University of Technology Chongqing 401121China

At present,the emerging solid-phase friction-based additive manufacturing technology,including friction rolling additive man-ufacturing(FRAM),can only manufacture simple single-pass *** this study,multi-layer multi-pass FRAM-deposited alumin-um alloy samples were successfully prepared using a non-shoulder tool *** material flow behavior and microstructure of the over-lapped zone between adjacent layers and passes during multi-layer multi-pass FRAM deposition were studied using the hybrid 6061 and 5052 aluminum *** results showed that a mechanical interlocking structure was formed between the adjacent layers and the adja-cent passes in the overlapped center *** friction and rolling of the tool head led to different degrees of lateral flow and plastic deformation of the materials in the overlapped zone,which made the recrystallization degree in the left and right edge zones of the over-lapped zone the highest,followed by the overlapped center zone and the non-overlapped *** tensile strength of the overlapped zone exceeded 90%of that of the single-pass deposition *** is proved that although there are uneven grooves on the surface of the over-lapping area during multi-layer and multi-pass deposition,they can be filled by the flow of materials during the deposition of the next lay-er,thus ensuring the dense microstructure and excellent mechanical properties of the overlapping *** multi-layer multi-pass FRAM deposition overcomes the limitation of deposition width and lays the foundation for the future deposition of large-scale high-performance components.

关键词： aluminum alloy additive manufacturing solid-state friction stir welding multi-layer multi-pass

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Superhydrophobic and corrosion-resistant siloxane-modified MgAl-LDHs coatings on magnesium alloy prepared under mild conditions

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International Journal of Minerals,Metallurgy and Materials 2025年第2期32卷 450-463页

作者： Wenxi Zhang Zhangzelong Zhuo Dan Xu Liang Wu Zhihui xie Chemical Synthesis and Pollution Control Key Laboratory of Sichuan Province College of Chemistry and Chemical EngineeringChina West Normal UniversityNanchong 637002China College of Materials Science and Engineering/National Engineering Research Center for Magnesium Alloys Chongqing UniversityChongqing 400044China

We have developed a superhydrophobic and corrosion-resistant LDH-W/PFDTMS composite coating on the surface of Mg *** composite comprised a tungstate-intercalated(LDH-W)underlayer that was grown at low temperature(relative to hydrothermal reaction conditions)under atmospheric pressure and an outer polysiloxane layer created from a solution containing perfluorodecyltrimethoxysilane(PFDTMS)using a simple immersion *** successful intercalation of tungstate into the LDH phase and the following formation of the polysiloxane layer were confirmed through X-ray diffraction(XRD),Fourier transform infrared(FTIR)spectroscopy,and X-ray photoelectron spectroscopy(XPS).The corrosion resistance of the LDH-W film,both before and after the PFDTMS modification,was evaluated using electrochemical impedance spectroscopy(EIS),Tafel curves,and immersion *** results showed that Mg coated with LDH-W/PFDTMS exhibited significantly enhanced corrosion protection compared to the unmodified LDHW film,with no apparent signs of corrosion after exposure to 3.5wt%NaCl solution for 15 ***,the LDH-W/PFDTMS coating demonstrated superior superhydrophobicity and self-cleaning properties against water and several common beverages,as confirmed by static contact angle and water-repellency *** results offer valuable insights into preparing superhydrophobic and corrosion-resistant LDH-based composite coatings on Mg alloy surfaces under relatively mild reaction conditions.

关键词： Mg alloy corrosion coating layered double hydroxide

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Unraveling the significance of cobalt on transformation kinetics,crystallography and impact toughness in high-strength steels

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International Journal of Minerals,Metallurgy and Materials 2025年第2期32卷 380-390页

作者： Yishuang Yu Jingxiao Zhao Xuelin Wang Hui Guo Zhenjia xie Chengjia Shang Collaborative Innovation Center of Steel Technology University of Science and Technology BeijingBeijing 100083China School of Materials Science and Engineering Shanghai Jiao Tong UniversityShanghai 200240China State Key Laboratory for Advanced Metals and Materials University of Science and Technology BeijingBeijing 100083China

This work reveals the significant effects of cobalt(Co)on the microstructure and impact toughness of as-quenched highstrength steels by experimental characterizations and thermo-kinetic *** results show that the Co-bearing steel exhibits finer blocks and a lower ductile-brittle transition temperature than the steel without ***,the Co-bearing steel reveals higher transformation rates at the intermediate stage with bainite volume fraction ranging from around 0.1 to *** improved impact toughness of the Co-bearing steel results from the higher dense block boundaries dominated by the V1/V2 variant ***,the addition of Co induces a larger transformation driving force and a lower bainite start temperature(BS),thereby contributing to the refinement of blocks and the increase of the V1/V2 variant *** findings would be instructive for the composition,microstructure design,and property optimization of high-strength steels.

关键词： high-strength steel cobalt transformation kinetics crystallography impact toughness

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Local-contrastive-learning machine with both generalization and adversarial robustness: A statistical physics analysis

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Science China(Physics,Mechanics & Astronomy) 2025年第1期Mechanics & Astronomy) .卷 109-123页

作者： Mingshan xie Yuchen Wang Haiping Huang PMI Lab School of Physics Sun Yat-sen University Guangdong Provincial Key Laboratory of Magnetoelectric Physics and Devices Sun Yat-sen University

Distinct from human cognitive processing, deep neural networks trained by backpropagation can be easily fooled by adversarial examples. To design a semantically meaningful representation learning, we discard backpropagation, and instead, propose a local contrastive learning, where the representations for the inputs bearing the same label shrink(akin to boson) in hidden layers,while those of different labels repel(akin to fermion). This layer-wise learning is local in nature, being biologically plausible.A statistical mechanics analysis shows that the target fermion-pair-distance is a key parameter. Moreover, the application of this local contrastive learning to MNIST benchmark dataset demonstrates that the adversarial vulnerability of standard perceptron can be greatly mitigated by tuning the target distance, i.e., controlling the geometric separation of prototype manifolds.

关键词： machine learning statistical mechanics adversarial robustness neural networks

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