Mass spectrometry imaging(MSI)has made the spatio-chemical characterization of a broad range of small-molecule metabolites within biological tissues possible.However,available matrix-assisted laser desorption/ionizati...Mass spectrometry imaging(MSI)has made the spatio-chemical characterization of a broad range of small-molecule metabolites within biological tissues possible.However,available matrix-assisted laser desorption/ionization mass spectrometry(MALDI-MS)suffers from severe background interferences in low-mass ranges and inhomogeneous matrix deposition.Thus,surface-assisted LDI-MS(SALDI-MS)has been an attractive alternative for high-sensitivity detection and imaging of small biomolecules.In this study,we construct a new composite substrate,hydrophobic polydopamine(hPDA)-modified TiO_(2)nanotube(TDNT)coated with plasmonic gold nanoparticle(AuNP-hPDA-TDNT),as a dual-polarity SALDI substrate using an easy and cost-effective fabrication approach.Benefitting from the synergistic effects of TDNT semiconductor and plasmonic PDA modification,this SALDI substrate exhibits superior performance for dual-polarity detection of a vast diversity of small molecules.Highly reduced background interferences,lower detection limits,and spot-to-spot repeatability can be achieved using AuNP-hPDA-TDNT substrates.Due to its unique imprinting performance,various metabolites and lipids can be visualized within jatropha integerrima petals,ginkgo leaves,strawberry fruits,and latent fingerprints.More valuably,the universality of this matrix-free substrate is demonstrated for mapping spatial distribution of lipids within mouse brain tissue sections.Considered together,this AuNP-hPDA-TDNT material is expected to be a promising SALDI substrate in various fields,especially in nanomaterial development and life sciences.展开更多
Design and discovery of carrier-mediated modified pesticides are vital for reducing pesticide dosage and increasing utilization,yet it remains a great challenge due to limited insights into plant translocation mechani...Design and discovery of carrier-mediated modified pesticides are vital for reducing pesticide dosage and increasing utilization,yet it remains a great challenge due to limited insights into plant translocation mechanisms.Nanostructure/nanoparticle assisted laser desorption/ionization strategy has established itself as a preferential analytical tool for biological tissue analysis,whereas potential applications in plant sciences are hindered with regard to the inability to slice plant leaves and petals.Herein,we report gold nanoparticle(AuNP)-immersed paper imprinting mass spectrometry imaging(MSI)for the spatiotemporal visualization of pesticide translocation in plant leaves.This approach plays a dual role in preserving spatial information and improving ionization efficiency for pesticides regardless of imaging artifacts due to homogenous AuNP deposition.Using this MSI platform,we proposed the elaborate plant translocation mechanism of agrochemicals for the first time,which is currently poorly understood.The dynamic processes of carrier-mediated pesticides can be clearly visualized,including crossing of plasma membranes by transporters,translocation downward in stems through the phloem,diffusion to the xylem and,conversely,accumulation at margins of the treated leaves.Moreover,this AuNP-assisted paper imprinting method could be highly compatible with laser-based MSI instruments,expediting researches across a broad range of fields,especially in nanomaterial development and life sciences.展开更多
Telomerase plays an essential role in many biological processes.DNA methylation regulates the expression of many genes,including telomerase.Here,we propose a deformable satellite nanocapsule fluorescein isothiocyanate...Telomerase plays an essential role in many biological processes.DNA methylation regulates the expression of many genes,including telomerase.Here,we propose a deformable satellite nanocapsule fluorescein isothiocyanate(FITC)-hollowbowl mesoporous organicsilica@gold nanoparticles-methyl-CpG-binding protein 2(MECP 2)-silver nanoclusters(FHBMO@AMA),for simultaneous quantitative detection of both cytoplasmic telomerase activity and the degree of DNA methylation.This strategy enabled spatial-based detection in cells.The total cytoplasmic telomerase activity was detected by fluorescence energy resonance transfer(FRET)between FHBMO and gold nanoparticles(Au NPs),while the DNA methylation in the nucleus was detected by enhanced fluorescence of silver nanoclusters(Ag NCs).Furthermore,FHBMO@AMA could intuitively distinguish between the differences in telomerase expression in cells during the DNA synthesis period at the mitotic phase(S/M)of the cell cycle.Interestingly,the ratio of the two detections(telomerase activity/DNA methylation)significantly correlated with the efficacy of anticancer drugs.At the same time,there was no apparent linear relationship between any single detection target and the efficacy of the anticancer drugs.Therefore,based on the relationship between telomerase activity and DNA methylation,our newly developed approach serves as new and feasible method for evaluating the efficacy of anticancer drugs,thereby,extending the technology toolbox for precision in medical and pharmaceutical analysis of drug potency.展开更多
基金the National Natural Science Foundation of China(Nos.31901911 and 21904142)the Natural Science Foundation of Guangdong Province(Nos.2019A1515011521 and 2022A1515011385)supported by the Young Talent Support Project of Guangzhou Association for Science and Technology(No.QT20220101031).
文摘Mass spectrometry imaging(MSI)has made the spatio-chemical characterization of a broad range of small-molecule metabolites within biological tissues possible.However,available matrix-assisted laser desorption/ionization mass spectrometry(MALDI-MS)suffers from severe background interferences in low-mass ranges and inhomogeneous matrix deposition.Thus,surface-assisted LDI-MS(SALDI-MS)has been an attractive alternative for high-sensitivity detection and imaging of small biomolecules.In this study,we construct a new composite substrate,hydrophobic polydopamine(hPDA)-modified TiO_(2)nanotube(TDNT)coated with plasmonic gold nanoparticle(AuNP-hPDA-TDNT),as a dual-polarity SALDI substrate using an easy and cost-effective fabrication approach.Benefitting from the synergistic effects of TDNT semiconductor and plasmonic PDA modification,this SALDI substrate exhibits superior performance for dual-polarity detection of a vast diversity of small molecules.Highly reduced background interferences,lower detection limits,and spot-to-spot repeatability can be achieved using AuNP-hPDA-TDNT substrates.Due to its unique imprinting performance,various metabolites and lipids can be visualized within jatropha integerrima petals,ginkgo leaves,strawberry fruits,and latent fingerprints.More valuably,the universality of this matrix-free substrate is demonstrated for mapping spatial distribution of lipids within mouse brain tissue sections.Considered together,this AuNP-hPDA-TDNT material is expected to be a promising SALDI substrate in various fields,especially in nanomaterial development and life sciences.
基金support from the National Natural Science Foundation of China(Nos.31901911 and 21904142)the National Key R&D Program of China(No.2018YFD0200300)+1 种基金the Natural Science Foundation of Guangdong Province(No.2018A030310215)This work is also supported by the project funded by the National Postdoctoral Program for Innovative Talents(No.BX20180399).
文摘Design and discovery of carrier-mediated modified pesticides are vital for reducing pesticide dosage and increasing utilization,yet it remains a great challenge due to limited insights into plant translocation mechanisms.Nanostructure/nanoparticle assisted laser desorption/ionization strategy has established itself as a preferential analytical tool for biological tissue analysis,whereas potential applications in plant sciences are hindered with regard to the inability to slice plant leaves and petals.Herein,we report gold nanoparticle(AuNP)-immersed paper imprinting mass spectrometry imaging(MSI)for the spatiotemporal visualization of pesticide translocation in plant leaves.This approach plays a dual role in preserving spatial information and improving ionization efficiency for pesticides regardless of imaging artifacts due to homogenous AuNP deposition.Using this MSI platform,we proposed the elaborate plant translocation mechanism of agrochemicals for the first time,which is currently poorly understood.The dynamic processes of carrier-mediated pesticides can be clearly visualized,including crossing of plasma membranes by transporters,translocation downward in stems through the phloem,diffusion to the xylem and,conversely,accumulation at margins of the treated leaves.Moreover,this AuNP-assisted paper imprinting method could be highly compatible with laser-based MSI instruments,expediting researches across a broad range of fields,especially in nanomaterial development and life sciences.
基金The authors gratefully acknowledge the financial support from the National Natural Science Foundation of China(nos.21834004 and 21904063)the Natural Science Foundation of Jiangsu Province(no.BK20190279).
文摘Telomerase plays an essential role in many biological processes.DNA methylation regulates the expression of many genes,including telomerase.Here,we propose a deformable satellite nanocapsule fluorescein isothiocyanate(FITC)-hollowbowl mesoporous organicsilica@gold nanoparticles-methyl-CpG-binding protein 2(MECP 2)-silver nanoclusters(FHBMO@AMA),for simultaneous quantitative detection of both cytoplasmic telomerase activity and the degree of DNA methylation.This strategy enabled spatial-based detection in cells.The total cytoplasmic telomerase activity was detected by fluorescence energy resonance transfer(FRET)between FHBMO and gold nanoparticles(Au NPs),while the DNA methylation in the nucleus was detected by enhanced fluorescence of silver nanoclusters(Ag NCs).Furthermore,FHBMO@AMA could intuitively distinguish between the differences in telomerase expression in cells during the DNA synthesis period at the mitotic phase(S/M)of the cell cycle.Interestingly,the ratio of the two detections(telomerase activity/DNA methylation)significantly correlated with the efficacy of anticancer drugs.At the same time,there was no apparent linear relationship between any single detection target and the efficacy of the anticancer drugs.Therefore,based on the relationship between telomerase activity and DNA methylation,our newly developed approach serves as new and feasible method for evaluating the efficacy of anticancer drugs,thereby,extending the technology toolbox for precision in medical and pharmaceutical analysis of drug potency.