Exploring the Reaction Mechanisms of Fast Pyrolysis of Xylan Model Compounds via Tandem Mass Spectrometry and Quantum Chemical Calculations.
Zaikuan Josh YuPriya MurriaMckay W EastonJohn C DegensteinHanyu ZhuLan XuRakesh AgrawalW Nicholas DelgassFabio H RibeiroHilkka I KenttämaaPublished in: The journal of physical chemistry. A (2019)
A commercial fast pyrolysis probe coupled with a high-resolution tandem mass spectrometer was employed to identify the initial reactions and products of fast pyrolysis of xylobiose and xylotriose, model compounds of xylans. Fragmentation of the reducing end by loss of an ethenediol molecule via ring-opening and retro-aldol condensation was found to be the dominant pyrolysis pathway for xylobiose, and the structure of the product-β-d-xylopyranosylglyceraldehyde-was identified by comparing collision-activated dissociation of the ionized product and an ionized authentic compound. This intermediate can undergo further decomposition via the loss of formaldehyde to form β-d-xylopyranosylglycolaldehyde. In addition, the mechanisms of reactions leading to the loss of a water molecule or dissociation of the glycosidic linkages were explored computationally. These reactions are proposed to occur via pinacol ring contraction and/or Maccoll elimination mechanisms.
Keyphrases
- tandem mass spectrometry
- high resolution
- sewage sludge
- ultra high performance liquid chromatography
- municipal solid waste
- high performance liquid chromatography
- liquid chromatography
- gas chromatography
- molecular dynamics
- simultaneous determination
- mass spectrometry
- electron transfer
- density functional theory
- solid phase extraction
- anaerobic digestion
- molecular dynamics simulations
- high speed
- single molecule