Title: Radical–radical reactions, pyrene nucleation, and incipient soot formation in combustion

Abstract

Here, we present a combined experimental and probabilistic simulation study of soot-precursor. The experiments were conducted using aerosol mass spectrometry coupled with tunable vacuum ultraviolet radiation from the Advanced Light Source at Lawrence Berkeley National Laboratory. Mass spectra and photoionization efficiency (PIE) curves of soot precursor species were measured at different heights in a premixed flat flame and in a counter-flow diffusion flame fueled by ethylene and oxygen. The PIE curves at the pyrene mass from these flames were compared with reference PIE scans recorded for pyrene. The results demonstrate that other C₁₆H₁₀ isomers than pyrene are major components among species condensed onto incipient soot in this study, which is in agreement with the simulations. Species with mass 202 u only have a high prevalence in incipient soot particles drawn from the premixed flame, but hydrocarbon species with sizes in the range 200-400 u are important to incipient-soot formation in both flames. The simulations predict that some species form through combination reactions involving relatively large radicals and bypass traditional molecular-growth pathways through addition of small hydrocarbon species. The experimental results support this prediction; they demonstrate that these species have higher relative abundances in particles formed close to the fuel outletmore » than smaller, lighter molecular species and indicate that these species are important to early formation of incipient-soot precursors. The results also imply that a leading role in incipient-soot precursor formation is played by species with lower thermal stability than the even-carbon numbered, unsubstituted polycyclic aromatic hydrocarbons known as "stabilomers".« less

Authors:

Johansson, K. Olof ^[1]; Dillstrom, Tyler ^[2]; Elvati, Paolo  ^[2];

• Search DOE PAGES for author "Elvati, Paolo"
• Search DOE PAGES for ORCID "0000-0002-6882-6023"

Campbell, Matthew F. ^[1]; Schrader, Paul E. ^[1]; Popolan-Vaida, Denisia M. ^[3]; Richards-Henderson, Nicole K. ^[4]; Wilson, Kevin R. ^[4]; Violi, Angela  ^[2];

• Search DOE PAGES for author "Violi, Angela"
• Search DOE PAGES for ORCID "0000-0001-9517-668X"

Michelsen, Hope A. ^[1]

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+ Show Author Affiliations

1. Sandia National Laboratory (SNL-CA), Livermore, CA (United States)
2. University of Michigan, Ann Arbor, MI (United States)
3. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States)
4. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Publication Date:

Wed Oct 12 00:00:00 EDT 2016

Research Org.:

Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE National Nuclear Security Administration (NNSA); Alexander von Humboldt Foundation

OSTI Identifier:

1379642

Alternate Identifier(s):

OSTI ID: 1397903

Grant/Contract Number:  

AC02-05CH11231; AC04-94AL85000; SC0002619; AC04-94-AL85000

Resource Type:

Accepted Manuscript

Journal Name:

Proceedings of the Combustion Institute

Additional Journal Information:

Journal Volume: 36; Journal Issue: 1; Journal ID: ISSN 1540-7489

Publisher:

Elsevier

Country of Publication:

United States

Language:

English

Subject:

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; incipient soot; ethylene flame; PAH; radical reactions; pyrene