期刊
SCIENCE
卷 361, 期 6406, 页码 997-+出版社
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.aat3417
关键词
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资金
- U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences (BES), Chemical Sciences, Geosciences, and Biosciences Division, Gas Phase Chemical Physics Program
- Gas Phase Chemical Physics Program [DE-AC02-05CH11231]
- DOE BES [DE-AC02-05CH11231]
- DOE's National Nuclear Security Administration [DE-NA0003525]
Mystery surrounds the transition from gas-phase hydrocarbon precursors to terrestrial soot and interstellar dust, which are carbonaceous particles formed under similar conditions. Although polycyclic aromatic hydrocarbons (PAHs) are known precursors to high-temperature carbonaceous-particle formation, the molecular pathways that initiate particle formation are unknown. We present experimental and theoretical evidence for rapid molecular clustering-reaction pathways involving radicals with extended conjugation. These radicals react with other hydrocarbon species to form covalently bound complexes that promote further growth and clustering by regenerating resonance-stabilized radicals through low-barrier hydrogen-abstraction and hydrogen-ejection reactions. Such radical-chain reaction pathways may lead to covalently bound clusters of PAHs and other hydrocarbons that would otherwise be too small to condense at high temperatures, thus providing the key mechanistic steps for rapid particle formation and surface growth by hydrocarbon chemisorption.
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