Metal-organic frameworks(MOFs)combined with specific ligands are highly adaptable smart materials that can respond to external and physiological stimuli.In this study,we introduced a pyridinyl zwitterionic ligand with...Metal-organic frameworks(MOFs)combined with specific ligands are highly adaptable smart materials that can respond to external and physiological stimuli.In this study,we introduced a pyridinyl zwitterionic ligand with light/pH dual response into magnetic MOF composite(Fe_(3)O_(4)@ZW-MOF)for enrichment of phosphorylated peptides for the first time.The introduction of the developed ligand gives MOF material dual response properties.Light stimulation affects the generation/disappearance of free radicals of the pyridine derivative,resulting in a change in the charge gradient of the zwitterion,and zwitterion can also regulate the p H of the solution by adding acid or base.Therefore,the reversible capture and release of phosphorylated peptides can be easily achieved by adjusting light and pH.The established phosphorylated peptide enrichment platform exhibits high sensitivity(detection limit of 1 fmol),high selectivity(β-casein:BSA,1:1000),and good reusability(7 cycles).In addition,the method was applied to the enrichment of phosphorylated peptides in complex systems(non-fat milk and human serum),demonstrating the feasibility of this method for phosphoproteom analysis.In conclusion,the synthesized Fe_(3)O_(4)@ZW-MOF is a promising MOF material,which provides the possibility to advance the application of responsive MOFs materials in proteomics.展开更多
Investigations of glycosylated proteins or peptides and their related biological pathways provide new possibilities for illuminating the physiological and pathological mechanisms of glycosylation modification.However,...Investigations of glycosylated proteins or peptides and their related biological pathways provide new possibilities for illuminating the physiological and pathological mechanisms of glycosylation modification.However,open-ended and in-depth analysis of glycoproteomics is usually subjected to the low-abundance of glycopeptides,heterogeneous glycans,and a variety of interference molecules.In order to alleviate the influence of these obstacles,effective preconcentration of glycopeptides are indispensable.Here,we employed a hydrophilic interaction liquid chromatography(HILIC)-based method to universally capture glycopeptides.Glutathione modified magnetic nanoparticles(Fe304@AuGSH) were synthesized through a simple process and exploited to enrich glycopeptides from complex samples.The prepared materials showed excellent ability to trap glycopeptides from standard glycoproteins digests,low detection limit(10 fmol/p L),and good selectivity(HRP:BSA=1:100).These results indicated that glutathione-based magnetic nanoparticles synthesized in this work had great potential for glycopeptides enrichment.展开更多
基金the financial support of the Fundamental Research Funds for the Central Universities,JLU,ChinaOpen Project of State Key Laboratory of Supramolecular Structure and Materials,Jilin University,China(No.sklssm2022012)。
文摘Metal-organic frameworks(MOFs)combined with specific ligands are highly adaptable smart materials that can respond to external and physiological stimuli.In this study,we introduced a pyridinyl zwitterionic ligand with light/pH dual response into magnetic MOF composite(Fe_(3)O_(4)@ZW-MOF)for enrichment of phosphorylated peptides for the first time.The introduction of the developed ligand gives MOF material dual response properties.Light stimulation affects the generation/disappearance of free radicals of the pyridine derivative,resulting in a change in the charge gradient of the zwitterion,and zwitterion can also regulate the p H of the solution by adding acid or base.Therefore,the reversible capture and release of phosphorylated peptides can be easily achieved by adjusting light and pH.The established phosphorylated peptide enrichment platform exhibits high sensitivity(detection limit of 1 fmol),high selectivity(β-casein:BSA,1:1000),and good reusability(7 cycles).In addition,the method was applied to the enrichment of phosphorylated peptides in complex systems(non-fat milk and human serum),demonstrating the feasibility of this method for phosphoproteom analysis.In conclusion,the synthesized Fe_(3)O_(4)@ZW-MOF is a promising MOF material,which provides the possibility to advance the application of responsive MOFs materials in proteomics.
基金supported by Jilin Provincial Science & Technology Department(No.20190201079JC)the Fundamental Research Funds for the Central Universities,JLUOpen Project of State Key Laboratory of Supramolecular Structure and Materials, Jilin University,China(No.sklssm2019020)
文摘Investigations of glycosylated proteins or peptides and their related biological pathways provide new possibilities for illuminating the physiological and pathological mechanisms of glycosylation modification.However,open-ended and in-depth analysis of glycoproteomics is usually subjected to the low-abundance of glycopeptides,heterogeneous glycans,and a variety of interference molecules.In order to alleviate the influence of these obstacles,effective preconcentration of glycopeptides are indispensable.Here,we employed a hydrophilic interaction liquid chromatography(HILIC)-based method to universally capture glycopeptides.Glutathione modified magnetic nanoparticles(Fe304@AuGSH) were synthesized through a simple process and exploited to enrich glycopeptides from complex samples.The prepared materials showed excellent ability to trap glycopeptides from standard glycoproteins digests,low detection limit(10 fmol/p L),and good selectivity(HRP:BSA=1:100).These results indicated that glutathione-based magnetic nanoparticles synthesized in this work had great potential for glycopeptides enrichment.