دورية أكاديمية

Time resolved growth of (N)-polycyclic aromatic hydrocarbons in engine deposits uncovered with OrbiSIMS depth profiling.

التفاصيل البيبلوغرافية
العنوان: Time resolved growth of (N)-polycyclic aromatic hydrocarbons in engine deposits uncovered with OrbiSIMS depth profiling.
المؤلفون: Edney MK; Department of Chemical and Environmental Engineering, Faculty of Engineering, University of Nottingham, University Park, Nottingham, NG7 7RD, UK., He W; School of Pharmacy, University of Nottingham, University Park, Nottingham, NG7 2RD, UK. david.scurr@nottingham.ac.uk., Smith EF; Department of Chemistry, University of Nottingham, University Park, Nottingham, NG7 2RD, UK., Wilmot E; Innospec Ltd., Oil Sites Road, Ellesmere Port, Cheshire, CH65 4EY, UK., Reid J; Innospec Ltd., Oil Sites Road, Ellesmere Port, Cheshire, CH65 4EY, UK., Barker J; Innospec Ltd., Oil Sites Road, Ellesmere Port, Cheshire, CH65 4EY, UK., Griffiths RL; School of Pharmacy, University of Nottingham, University Park, Nottingham, NG7 2RD, UK. david.scurr@nottingham.ac.uk., Alexander MR; School of Pharmacy, University of Nottingham, University Park, Nottingham, NG7 2RD, UK. david.scurr@nottingham.ac.uk., Snape CE; Department of Chemical and Environmental Engineering, Faculty of Engineering, University of Nottingham, University Park, Nottingham, NG7 7RD, UK., Scurr DJ; School of Pharmacy, University of Nottingham, University Park, Nottingham, NG7 2RD, UK. david.scurr@nottingham.ac.uk.
المصدر: The Analyst [Analyst] 2022 Aug 22; Vol. 147 (17), pp. 3854-3866. Date of Electronic Publication: 2022 Aug 22.
نوع المنشور: Journal Article
اللغة: English
بيانات الدورية: Publisher: Royal Society of Chemistry Country of Publication: England NLM ID: 0372652 Publication Model: Electronic Cited Medium: Internet ISSN: 1364-5528 (Electronic) Linking ISSN: 00032654 NLM ISO Abbreviation: Analyst Subsets: MEDLINE
أسماء مطبوعة: Publication: Cambridge : Royal Society of Chemistry
Original Publication: London : Chemical Society
مواضيع طبية MeSH: Air Pollutants*/analysis , Air Pollution*/analysis , Polycyclic Aromatic Hydrocarbons*/analysis, Hydrocarbons/analysis ; Vehicle Emissions/analysis
مستخلص: Carbonaceous 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 mass resolving power capabilities of 3D Orbitrap secondary ion mass spectrometry (3D OrbiSIMS) argon cluster 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 C 2 H 2 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.
المشرفين على المادة: 0 (Air Pollutants)
0 (Hydrocarbons)
0 (Polycyclic Aromatic Hydrocarbons)
0 (Vehicle Emissions)
تواريخ الأحداث: Date Created: 20220729 Date Completed: 20220823 Latest Revision: 20220823
رمز التحديث: 20221213
DOI: 10.1039/d2an00798c
PMID: 35904202
قاعدة البيانات: MEDLINE
الوصف
تدمد:1364-5528
DOI:10.1039/d2an00798c