Pyrene synthesis in circumstellar envelopes and its role in the formation of 2D nanostructures
Abstract
For the past decades, the hydrogen-abstraction/acetylene-addition (HACA) mechanism has been instrumental in attempting to untangle the origin of polycyclic aromatic hydrocarbons (PAHs) as identified in carbonaceous meteorites such as Allende and Murchison. However, the fundamental reaction mechanisms leading to the synthesis of PAHs beyond phenanthrene (C14H10) are still unknown. By exploring the reaction of the 4-phenanthrenyl radical (C14H9•) with acetylene (C2H2) under conditions prevalent in carbon-rich circumstellar environments, we show evidence of a facile, isomer-selective formation of pyrene (C16H10). Along with the hydrogen-abstraction/vinylacetylene-addition (HAVA) mechanism, molecular mass growth processes from pyrene may lead through systematic ring expansions not only to more complex PAHs, but ultimately to 2D graphene-type structures. These fundamental reaction mechanisms are crucial to facilitate an understanding of the origin and evolution of the molecular universe and, in particular, of carbon in our Galaxy.
- Authors:
-
[2];
[2];
- Univ. of Hawaii at Manoa, Honolulu, HI (United States). Dept. of Chemistry
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division
- Univ. of California, Berkeley, CA (United States). Dept. of Chemistry; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division; Univ. of California, Berkeley, CA (United States). Kavli Energy Nano Sciences Inst.
- Florida International Univ., Miami, FL (United States). Dept. of Chemistry and Biochemistry
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Univ. of Hawaii at Manoa, Honolulu, HI (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
- OSTI Identifier:
- 1461139
- Alternate Identifier(s):
- OSTI ID: 1603085
- Grant/Contract Number:
- AC02-05CH11231; FG02-03ER15411
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Astronomy
- Additional Journal Information:
- Journal Volume: 2; Journal Issue: 5; Journal ID: ISSN 2397-3366
- Publisher:
- Springer
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 79 ASTRONOMY AND ASTROPHYSICS
Citation Formats
Zhao, Long, Kaiser, Ralf I., Xu, Bo, Ablikim, Utuq, Ahmed, Musahid, Joshi, Dharati, Veber, Gregory, Fischer, Felix R., and Mebel, Alexander M. Pyrene synthesis in circumstellar envelopes and its role in the formation of 2D nanostructures. United States: N. p., 2018.
Web. doi:10.1038/s41550-018-0399-y.
Zhao, Long, Kaiser, Ralf I., Xu, Bo, Ablikim, Utuq, Ahmed, Musahid, Joshi, Dharati, Veber, Gregory, Fischer, Felix R., & Mebel, Alexander M. Pyrene synthesis in circumstellar envelopes and its role in the formation of 2D nanostructures. United States. https://doi.org/10.1038/s41550-018-0399-y
Zhao, Long, Kaiser, Ralf I., Xu, Bo, Ablikim, Utuq, Ahmed, Musahid, Joshi, Dharati, Veber, Gregory, Fischer, Felix R., and Mebel, Alexander M. Mon .
"Pyrene synthesis in circumstellar envelopes and its role in the formation of 2D nanostructures". United States. https://doi.org/10.1038/s41550-018-0399-y. https://www.osti.gov/servlets/purl/1461139.
@article{osti_1461139,
title = {Pyrene synthesis in circumstellar envelopes and its role in the formation of 2D nanostructures},
author = {Zhao, Long and Kaiser, Ralf I. and Xu, Bo and Ablikim, Utuq and Ahmed, Musahid and Joshi, Dharati and Veber, Gregory and Fischer, Felix R. and Mebel, Alexander M.},
abstractNote = {For the past decades, the hydrogen-abstraction/acetylene-addition (HACA) mechanism has been instrumental in attempting to untangle the origin of polycyclic aromatic hydrocarbons (PAHs) as identified in carbonaceous meteorites such as Allende and Murchison. However, the fundamental reaction mechanisms leading to the synthesis of PAHs beyond phenanthrene (C14H10) are still unknown. By exploring the reaction of the 4-phenanthrenyl radical (C14H9•) with acetylene (C2H2) under conditions prevalent in carbon-rich circumstellar environments, we show evidence of a facile, isomer-selective formation of pyrene (C16H10). Along with the hydrogen-abstraction/vinylacetylene-addition (HAVA) mechanism, molecular mass growth processes from pyrene may lead through systematic ring expansions not only to more complex PAHs, but ultimately to 2D graphene-type structures. These fundamental reaction mechanisms are crucial to facilitate an understanding of the origin and evolution of the molecular universe and, in particular, of carbon in our Galaxy.},
doi = {10.1038/s41550-018-0399-y},
journal = {Nature Astronomy},
number = 5,
volume = 2,
place = {United States},
year = {Mon Mar 05 00:00:00 EST 2018},
month = {Mon Mar 05 00:00:00 EST 2018}
}
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Figures / Tables:
Figure 1: Possible structures of isomers of aromatic molecules detected in carbonaceous meteorites. [1] biphenyl, [2] naphthalene, [3] anthracene, [4] phenanthrene, [5] triphenylene, [6] pyrene, [7] chrysene, [8] benz[a]anthracene, [9] benzo[a]pyrene, [10] benzo[e]pyrene.
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