期刊
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
卷 114, 期 31, 页码 8169-8174出版社
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1705463114
关键词
aromatics; oxidation; ozone; secondary organic aerosol; air pollution
资金
- National Natural Science Foundation of China [41675122, 41373102, 21577177, 41425015]
- Science and Technology Program of Guangzhou City [201707010188]
- Robert A. Welch Foundation [A-1417]
- Ministry of Science and Technology of China [2013CB955800]
- Texas AM University
- NASA Earth and Space Science Fellowship Program
- National Science Foundation Graduate Research Fellowship Program
- Texas A&M University Supercomputing Facilities
- Grants-in-Aid for Scientific Research [26410006] Funding Source: KAKEN
Photochemical oxidation of aromatic hydrocarbons leads to tropospheric ozone and secondary organic aerosol (SOA) formation, with profound implications for air quality, human health, and climate. Toluene is the most abundant aromatic compound under urban environments, but its detailed chemical oxidation mechanism remains uncertain. From combined laboratory experiments and quantum chemical calculations, we show a toluene oxidation mechanism that is different from the one adopted in current atmospheric models. Our experimental work indicates a largerthan-expected branching ratio for cresols, but a negligible formation of ring-opening products (e.g., methylglyoxal). Quantum chemical calculations also demonstrate that cresols are much more stable than their corresponding peroxy radicals, and, for the most favorable OH (ortho) addition, the pathway of H extraction by O-2 to form the cresol proceeds with a smaller barrier than O-2 addition to form the peroxy radical. Our results reveal that phenolic (rather than peroxy radical) formation represents the dominant pathway for toluene oxidation, highlighting the necessity to reassess its role in ozone and SOA formation in the atmosphere.
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