Abstract
RATIONALE: Selective derivatization of peptide
N-terminus with 4-formyl-benzenesulfonic acid (FBSA) enables
chemically activated fragmentation in ESI+/- (positive and negative ion
mode) under charge reduction conditions. Overlapped positive and
negative tandem mass spectra pinpoint b-ions making the assignment of
b-ion series fragments easy and accurate. METHODS: We developed
a FBSA-peptide microwave assisted derivatization procedure. Derivatized
and non-derivatized bovine serum albumin tryptic peptides and insulin
non-tryptic peptide were compared after MS/MS analysis in positive and
negative ion mode. High-quality dataset of sulfonated b-ions obtained in
negative tandem mass spectra of singly charged FBSA-peptides were
matched to detected b-ions in positive MS/MS spectra. Moreover, negative
spectra signals were converted and matched against y-ions in positive
tandem mass spectra to identify complete peptide sequences.
RESULTS: The FBSA derivatization procedure produced a
significantly improved MS/MS dataset (populated by high-intensity
signals of b- and y-ions) in comparison to commonly used
N-terminal sulfonation reagents. Undesired side reactions do not
occur and the procedure reduces the derivatization time. It was found
that b-ions comprise 15% and 13% of all fragment ions generated in
positive and negative ion mode, respectively. High visibility of b-ion
series in negative ion mode can be attributed to the N-terminal
sulfonation which had no effect on the production of b-ion series in
positive ion mode. CONCLUSIONS: The FBSA derivatization and
de novo sequencing approach outlined here provides a reliable
method for accurate peptide sequence assignment. Increased production of
the b-ions in positive and negative ion mode greatly improves peak
assignment and thus enables accurate sequence reconstruction.
Implementation of the named methodology would improve the quality of
de novo sequencing data and reduce the number of misinterpreted
spectra.