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dc.contributor.authorEdney, Max
dc.contributor.authorScurr, David
dc.contributor.otherHe, Wenshi
dc.contributor.otherSmith, Emily
dc.contributor.otherWilmot, Edward
dc.contributor.otherReid, Jacqueline
dc.contributor.otherBarker, Jim
dc.contributor.otherGriffiths, Rian
dc.contributor.otherAlexander, Morgan
dc.contributor.otherSnape, Colin
dc.description.abstractCarbonaceous deposits are ubiquitous, being formed on surfaces in engines, fuel systems and on catalysts operating at high temperatures for hydrocarbon transformations. In internal combustion engines, their formation negatively affects worldwide vehicle emissions and fuel economy, leading to premature deaths and environmental damage. Deposit composition and formation pathways are poorly understood due to their insolubility and the intrinsic complexity of their layered carbonaceous matrix. Here, we apply the in-situ high resolution analysis capabilities of 3D Orbitrap secondary ion mass spectrometry (3D OrbiSIMS) depth profiling on 16 lab grown deposits and evidence common molecular distributions in deposit depth and in positions relative to the combustion chamber. We observe the products of the growth of both planar and curved polycyclic aromatic hydrocarbons to form small fullerenes over time in the engine and propose possible formation pathways which explain the molecular distributions observed. These include alkyl scission, cyclisation of aliphatic side chains and hydrogen abstraction C2H2 addition to form larger aromatic structures. We apply this pathway to previously unidentified nitrogen containing structures in deposits including quinolines and carbazoles. For the first time, 3D OrbiSIMS results were compared and validated with data from atmospheric pressure matrix assisted laser desorption ionization MS. The comprehensive characterization provided will help the development of a new generation of chemical additives to reduce deposits, and thus improve vehicle emissions and global air quality.en_UK
dc.publisherUniversity of Nottinghamen_UK
dc.subject.lcshSecondary ion mass spectrometryen_UK
dc.subject.lcshPolycyclic aromatic hydrocarbonsen_UK
dc.titleTime resolved growth of (N)-polycyclic aromatic hydrocarbons in engine deposits uncovered with OrbiSIMS depth profilingen_UK
dc.subject.free3D OrbiSIMS, GCMS, engine depositsen_UK
dc.subject.jacsPhysical sciences::Chemistry::Organic chemistry::Organometallic chemistryen_UK
dc.subject.lcQ Science::QD Chemistryen_UK
dc.contributor.corporateInnospec Ltd.en_UK
uon.divisionUniversity of Nottingham, UK Campusen_UK
uon.funder.controlledEngineering & Physical Sciences Research Councilen_UK
uon.datatypeData on gasoline composition, 3D OrbiSIMS and XPS depth profiling data on depositsen_UK
uon.collectionmethodGC-MS analysis, 3D OrbiSIMSen_UK
uon.institutes-centresUniversity of Nottingham, UK Campusen_UK

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