Formation of H3O+ and OH by CO2 and N2O trace gases in the atmospheric environment

被引:3
作者
Catone, Daniele [1 ]
Castrovilli, Mattea Carmen [2 ]
Nicolanti, Francesca [3 ]
Satta, Mauro [4 ,5 ]
Cartoni, Antonella [5 ]
机构
[1] CNR, ISM, Area Ric Roma 2, Via Fosso Cavaliere 100, I-00133 Rome, Italy
[2] CNR, ISM, Area Ric Roma 1, I-00015 Monterotondo, Italy
[3] Sapienza Univ Rome, Dept Phys, Ple Aldo Moro 5, I-00185 Rome, Italy
[4] Sapienza Univ Rome, Dept Chem, CNR, ISMN, Ple Aldo Moro 5, I-00185 Rome, Italy
[5] Sapienza Univ Rome, Dept Chem, Ple Aldo Moro 5, I-00185 Rome, Italy
关键词
ION-MOLECULE REACTIONS; VIBRATIONAL-RELAXATION; WATER-VAPOR; STRATOSPHERE; INJECTION; CONSTANT;
D O I
10.1039/d3cp02427j
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The impact of cosmic rays' energetic subatomic particles on climate and global warming is still controversial and under debate. Cosmic rays produce ions that can trigger fast reactions affecting chemical networks in the troposphere and stratosphere especially when a large amount of relevant trace gases such as carbon dioxide, methane, sulfur dioxide and water are injected by volcanic eruptions. This work focuses on synchrotron experiments and an ab initio theoretical study of the ion chemistry of carbon dioxide and nitrous oxide radical cations reacting with water. These molecules catalyze a fast exothermic formation of hydronium ions H3O+ and the hydroxyl radical OH, the main oxidant in the atmosphere. Moreover, theoretical calculations demonstrate that at the end of the catalytic cycle, CO2 and N2O are produced vibrationally excited and subsequently they quench in the microsecond time scale by collision with the surrounding atmospheric molecules at the pressure and temperature of the upper-troposphere/stratosphere. The chemistry involved in these reactions has a strong impact on the oxidant capacity of the atmosphere, on the sulfate aerosol production, on the cloud formation and eventually on the chemical networks controlling climate and global warming models.
引用
收藏
页码:25619 / 25628
页数:10
相关论文
共 55 条
[41]   HITEMP, the high-temperature molecular spectroscopic database [J].
Rothman, L. S. ;
Gordon, I. E. ;
Barber, R. J. ;
Dothe, H. ;
Gamache, R. R. ;
Goldman, A. ;
Perevalov, V. I. ;
Tashkun, S. A. ;
Tennyson, J. .
JOURNAL OF QUANTITATIVE SPECTROSCOPY & RADIATIVE TRANSFER, 2010, 111 (15) :2139-2150
[42]  
Ruscic B., 2020, Active Thermochemical Tables (ATcT), version 1.176 of the Thermochemical Network
[43]  
Satta M., 2022, CONDENS MATTER, V46, P1
[44]   Ion Chemistry of Carbon Dioxide in Nonthermal Reaction with Molecular Hydrogen [J].
Satta, Mauro ;
Catone, Daniele ;
Castrovilli, Mattea Carmen ;
Bolognesi, Paola ;
Avaldi, Lorenzo ;
Zema, Nicola ;
Cartoni, Antonella .
JOURNAL OF PHYSICAL CHEMISTRY A, 2022, 126 (22) :3463-3471
[45]   The Reaction of Sulfur Dioxide Radical Cation with Hydrogen and its Relevance in Solar Geoengineering Models [J].
Satta, Mauro ;
Cartoni, Antonella ;
Catone, Daniele ;
Castrovilli, Mattea Carmen ;
Bolognesi, Paola ;
Zema, Nicola ;
Avaldi, Lorenzo .
CHEMPHYSCHEM, 2020, 21 (11) :1146-1156
[46]   A joint theoretical and experimental study on diiodomethane: Ions and neutrals in the gas phase [J].
Satta, Mauro ;
Bolognesi, Paola ;
Cartoni, Antonella ;
Casavola, Anna Rita ;
Catone, Daniele ;
Markus, Pal ;
Avaldi, Lorenzo .
JOURNAL OF CHEMICAL PHYSICS, 2015, 143 (24)
[47]   The unexpected radiative impact of the Hunga Tonga eruption of 15th January 2022 [J].
Sellitto, P. ;
Podglajen, A. ;
Belhadji, R. ;
Boichu, M. ;
Carboni, E. ;
Cuesta, J. ;
Duchamp, C. ;
Kloss, C. ;
Siddans, R. ;
Begue, N. ;
Blarel, L. ;
Jegou, F. ;
Khaykin, S. ;
Renard, J-B ;
Legras, B. .
COMMUNICATIONS EARTH & ENVIRONMENT, 2022, 3 (01)
[48]   Ambient and Modified Atmospheric Ion Chemistry: From Top to Bottom [J].
Shuman, Nicholas S. ;
Hunton, Donald E. ;
Viggiano, Albert A. .
CHEMICAL REVIEWS, 2015, 115 (10) :4542-4570
[49]   THE VIBRATIONAL DEACTIVATION OF THE (00(0)1) AND (01(1)0) - MODES OF CO2 MEASURED DOWN TO 140-K [J].
SIDDLES, RM ;
WILSON, GJ ;
SIMPSON, CJSM .
CHEMICAL PHYSICS, 1994, 189 (03) :779-791
[50]   The role of cosmic rays in the Earth's atmospheric processes [J].
Siingh, Devendraa ;
Singh, R. P. .
PRAMANA-JOURNAL OF PHYSICS, 2010, 74 (01) :153-168