Mass Spectrometry Sampling Under Ambient Conditions with Desorption Electrospray Ionization

A new method of desorption ionization is described and applied to the ionization of various compounds, including peptides and proteins present on metal, polymer, and mineral surfaces. Desorption electrospray ionization (DESI) is carried out by directing electrosprayed charged droplets and ions of solvent onto the surface to be analyzed. The impact of the charged particles on the surface produces gaseous ions of material originally present on the surface. The resulting mass spectra are similar to normal ESI mass spectra in that they show mainly singly or multiply charged molecular ions of the analytes. The DESI phenomenon was observed both in the case of conductive and insulator surfaces and for compounds ranging from nonpolar small molecules such as lycopene, the alkaloid coniceine, and small drugs, through polar compounds such as peptides and proteins. Changes in the solution that is sprayed can be used to selectively ionize particular compounds, including those in biological matrices. In vivo analysis is demonstrated.

[1]  Zachary Evenhouse,et al.  Supercritical fluids. , 1982, Environmental science & technology.

[2]  M. Stoeckli,et al.  Imaging mass spectrometry: A new technology for the analysis of protein expression in mammalian tissues , 2001, Nature Medicine.

[3]  S A Aksyonov,et al.  Impact desolvation of electrosprayed microdroplets--a new ionization method for mass spectrometry of large biomolecules. , 2001, Rapid communications in mass spectrometry : RCM.

[4]  F. Halgand,et al.  Tissue molecular ion imaging by gold cluster ion bombardment. , 2004, Analytical chemistry.

[5]  D. Cornett,et al.  Formation of multiply charged ions from large molecules using massive-cluster impact. , 1994, Rapid communications in mass spectrometry : RCM.

[6]  John B. Fenn,et al.  Electrospray ionization–principles and practice , 1990 .

[7]  C. Fenselau,et al.  Massive cluster impact ionization on a four sector tandem mass spectrometer , 1995 .

[8]  A. Wokaun,et al.  Nanoscale atmospheric pressure laser ablation-mass spectrometry. , 2001, Analytical chemistry.

[9]  M. Mann,et al.  Electrospray ionization for mass spectrometry of large biomolecules. , 1989, Science.

[10]  宁北芳,et al.  疟原虫var基因转换速率变化导致抗原变异[英]／Paul H, Robert P, Christodoulou Z, et al//Proc Natl Acad Sci U S A , 2005 .

[11]  A L Burlingame,et al.  Atmospheric pressure matrix-assisted laser desorption/ionization mass spectrometry. , 2000, Analytical chemistry.

[12]  R. Cotter,et al.  Atmospheric pressure MALDI/ion trap mass spectrometry. , 2000, Analytical chemistry.

[13]  D. Cornett,et al.  Matrix-free desorption of biomolecules using massive cluster impact. , 1994, Rapid communications in mass spectrometry : RCM.

[14]  H. W. Werner,et al.  Secondary Ion Mass Spectrometry: Basic Concepts, Instrumental Aspects, Applications and Trends , 1987 .

[15]  Terry D. Lee,et al.  Massive cluster impact mass spectrometry: a new desorption method for the analysis of large biomolecules. , 1991, Rapid communications in mass spectrometry : RCM.

[16]  C. Lebrilla,et al.  Evidence for enzymatic activity in the absence of solvent in gas-phase complexes of lysozyme and oligosaccharides , 1999 .

[17]  B. Cargile,et al.  Synthesis/degradation ratio mass spectrometry for measuring relative dynamic protein turnover. , 2004, Analytical chemistry.

[18]  Renato Zenobi,et al.  Quantitative determination of noncovalent binding interactions using soft ionization mass spectrometry , 2002 .

[19]  G. Siuzdak,et al.  Desorption–ionization mass spectrometry on porous silicon , 1999, Nature.

[20]  A. Appelhans,et al.  Static secondary ionization mass spectrometry and mass spectrometry/mass spectrometry (MS2) characterization of the chemical warfare agent HD on soil particle surfaces , 2001 .

[21]  A. Filippi,et al.  Gas-Phase Enantioselectivity , 2000 .

[22]  P. Chaurand,et al.  Organic ion imaging of biological tissue with secondary ion mass spectrometry and matrix-assisted laser desorption/ionization. , 2001, Journal of mass spectrometry : JMS.