Hiroshi Furutani | PubMed Health

PubMed2004

MALDI matrices for biomolecular analysis based on functionalized carbon nanomaterials.

When used in small molar ratios of matrix to analyte, derivatized fullerenes and single wall nanotubes are shown to be efficient matrices for matrix-assisted laser desorption/ionization (MALDI) mass spectrometry. The mixing of an acidic functionalized fullerene with a solution of bioanalyte, depositing a dried droplet, and irradiating with a pulsed nitrogen laser yields protonated or cationized molecular ions. Derivatized fullerenes could offer several advantages over conventional MALDI matrices: a high analyte ionization efficiency, a small molar ratios (less than 1) of matrix/analyte, and a broader optical absorption spectrum, which should obviate specific wavelength lasers for MALDI acquisitions. The major disadvantage to the use of fullerenes is the isobaric interference between matrix and analyte ions; however, it is overcome by using MALDI-ion mobility time-of-flight (IM-oTOF) mass spectrometry to preseparate carbon cluster ions from bioanalyte ions prior to TOF mass analysis. However, an alternative to the dried droplet preparation of fullerene MALDI samples is the aerosolization of matrix-analyte solutions (or slurries) followed by impacting the aerosol onto a stainless surface. We also demonstrate that the fullerene matrices can be used to acquire spectra from rat brain tissue.

Amino Acid Sequence↗

PubMed2004

Development and characterization of an aerosol time-of-flight mass spectrometer with increased detection efficiency.

This paper describes the development and characterization studies of a more efficient aerosol time-of-flight mass spectrometer (ATOFMS), showing results for the on-line detection and determination of the size and chemical composition of single fine (100-300 nm) and ultrafine (<100 nm) particles. An aerodynamic lens inlet was implemented, replacing the converging nozzle inlet used on conventional ATOFMS instruments. In addition, the light scattering region was modified to enhance the scattering signals for smaller particles. Polystyrene latex spheres (PSL) with aerodynamic diameters ranging from 95 to 290 nm were used to characterize the particle sizing efficiency (product of particle transmission efficiency and particle scattering efficiency), particle detection efficiency (product of particle sizing efficiency and particle hit rate), and particle beam profile and perform instrument calibration. At number concentrations of <20 particles/cm(3), the particle sizing efficiencies were determined to be approximately 0.5% for 95 nm and approximately 47% for 290-nm PSL particles, while the particle detection efficiencies were measured to be approximately 0.3% for 95 nm and 44% for 290-nm PSL particles. This represents a significant increase (i.e., at least 3 orders of magnitude) in detection efficiencies for smaller particles over the conventional ATOFMS. In addition, the beam profiles for PSL particles of various sizes were measured in the ion source of the mass spectrometer and follow a Gaussian distribution with a full width at half-maximum of approximately 0.35 mm. The resulting higher detection efficiencies allow ATOFMS to obtain higher temporal resolution measurements of the composition of fine and ultrafine individual particles as demonstrated in initial ambient measurements in La Jolla, CA. At typical ambient particle number concentrations of 10(2)-10(3) particles/cm(3), approximately 30 000 particles with aerodynamic diameters of <300 nm were detected with average 24-h hit rates of 30% for particles between 50 and 300 nm. This advancement, allowing for high temporal resolution measurements of the composition of smaller particles with higher efficiency, adds to a growing number of instruments that can chemically characterize individual fine and ultrafine particles, with the goal of providing new insights into a number of areas including environmental and material sciences, health effects studies, industrial hygiene, and national security.

Journal Article↗