Experimental observation of hydrocarbon growth by resonance stabilized radical-radical chain reaction

Couch, David Edward; Zhang, Angie J.; Taatjes, Craig A.; Hansen, Nils

doi:10.1002/ange.202110929

Experimental observation of hydrocarbon growth by resonance stabilized radical-radical chain reaction

Journal Article · Sun Oct 03 00:00:00 EDT 2021 · Angewandte Chemie

DOI:https://doi.org/10.1002/ange.202110929· OSTI ID:1827615

Couch, David Edward ^[1]; Zhang, Angie J. ^[1]; Taatjes, Craig A. ^[1]; Hansen, Nils ^[1]

Sandia National Lab. (SNL-CA), Livermore, CA (United States)

Rapid molecular weight growth of hydrocarbons occurs in flames, in industrial synthesis, and potentially in cold astrochemical environments. A variety of high- and low-temperature chemical mechanisms have been proposed and confirmed, but more facile pathways may be needed to explain observations. Here, we provide laboratory confirmation in a controlled pyrolysis environment of a recently proposed mechanism, radical-radical chain reactions of resonance-stabilized species. The recombination reaction of phenyl (c-C₆H₅) and benzyl (c-C₆H₅CH₂) radicals produces both diphenylmethane and diphenylmethyl radicals, the concentration of the latter increasing with rising temperature. A second phenyl addition to the product radical forms both triphenylmethane and triphenylmethyl radicals, confirming the propagation of radical-radical chain reactions under the experimental conditions of high temperature (1100-1600 K) and low pressure (~3 kPa). Similar chain reactions may contribute to particle growth in flames, the interstellar medium, and industrial reactors.

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: NA0003525

OSTI ID:: 1827615

Alternate ID(s):: OSTI ID: 1829775

Report Number(s):: SAND--2021-12501J; 700711

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie Journal Issue: 52 Vol. 133; ISSN 0044-8249

Publisher:: German Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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