This work investigates the use of ion mobility spectrometry and gas-phase infrared spectroscopy in combination with mass spectrometry for the structural analysis of isomeric sulfated glycans. Both methods have been successfully applied for the analysis of glycans before. Ion mobility spectrometry offers a structural dimension, missing in classical mass spectrometry for the differentiation of isomeric structures, while infrared spectroscopy can provide detailed structural information of even gas-phase conformations. These methods allowed for the investigation of the interaction of glycosaminoglycan with magnetic resonance imaging probes, revealing an intricate binding motive and a surprising dissociation behaviour. They allowed for the separation and quantification of twelve partially isomeric sulfated disaccharides, which previously were analyzed by tedious and time-consuming liquid chromatography methods. And finally, they revealed two unknown sulfated glycan-specific gas-phase rearrangement processes, which further consolidate the unique challenges faced in the structural analysis of sulfated glycans.
