Yali Li , Lei Zhu , Juan Li , Yuyang Chen , Luke M. Western , Dickon Young , Jens Mühle , Ray F. Weiss , Paul B. Krummel , Chris R. Lunder , Song Liu , Xicheng Li , Weitao Fu , Peng Zhang , Xue Zhang , Jiaming Zhang , Xingyi Wu , Yuchen Huang , Huizhong Shen , Jianhuai Ye , Xin Yang
{"title":"开发27种氟化温室气体(f -气体)的化学模块:GEOS-Chem中的反应,排放和实施","authors":"Yali Li , Lei Zhu , Juan Li , Yuyang Chen , Luke M. Western , Dickon Young , Jens Mühle , Ray F. Weiss , Paul B. Krummel , Chris R. Lunder , Song Liu , Xicheng Li , Weitao Fu , Peng Zhang , Xue Zhang , Jiaming Zhang , Xingyi Wu , Yuchen Huang , Huizhong Shen , Jianhuai Ye , Xin Yang","doi":"10.1016/j.atmosenv.2025.121604","DOIUrl":null,"url":null,"abstract":"<div><div>Fluorinated greenhouse gases (F-gases) are widely used in refrigeration, air-conditioning, semiconductor, and other industries, contributing a total direct radiative forcing only surpassed by carbon dioxide and methane. Current modeling efforts of F-gases use simplified chemical schemes and ignore three-dimensional dynamics, which limits the quantification of their chemical impacts, and a full suite of F-gases is not currently included in atmospheric chemical transport models. Here, we develop and implement a chemistry module in the GEOS-Chem model with 27 additional F-gases (including minor CFCs, minor HCFCs, HFCs, PFCs, SF<sub>6</sub>, NF<sub>3</sub>, and SO<sub>2</sub>F<sub>2</sub>) with constrained emissions. The updated simulations capture most of the surface mole fraction baseline trends and some pollution events for F-gases in 2020–2021, with a normalized mean bias between −14 % and 5 % at the Mace Head station and −17 % and 3 % at the ShangDianZi station. The impact of emission spatial distributions decreases with lifetime, suggesting that accurate global modeling of the background of long-lived species (>10 years) is less dependent on the spatial distribution of the emission than on the total magnitude. The impact of the updated simulation on key reactive species, including ozone, HO<sub><em>x</em></sub>, ClO<sub><em>x</em></sub>, and NO<sub><em>x</em></sub>, is <1 %. For species with 10-year lifetimes, F-gas chemical losses drive 20–40 % changes in their mixing ratios. Our work provides a comprehensive F-gases chemistry module complementing the major CFCs and HCFCs in the GEOS-Chem model, and this suite of F-gases provides potential applications for understanding their climate impacts and atmospheric processes.</div></div>","PeriodicalId":250,"journal":{"name":"Atmospheric Environment","volume":"363 ","pages":"Article 121604"},"PeriodicalIF":3.7000,"publicationDate":"2025-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Developing the chemistry module for 27 fluorinated greenhouse gases (F-gases): Reactions, emissions, and implementation in GEOS-Chem\",\"authors\":\"Yali Li , Lei Zhu , Juan Li , Yuyang Chen , Luke M. Western , Dickon Young , Jens Mühle , Ray F. Weiss , Paul B. Krummel , Chris R. Lunder , Song Liu , Xicheng Li , Weitao Fu , Peng Zhang , Xue Zhang , Jiaming Zhang , Xingyi Wu , Yuchen Huang , Huizhong Shen , Jianhuai Ye , Xin Yang\",\"doi\":\"10.1016/j.atmosenv.2025.121604\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Fluorinated greenhouse gases (F-gases) are widely used in refrigeration, air-conditioning, semiconductor, and other industries, contributing a total direct radiative forcing only surpassed by carbon dioxide and methane. Current modeling efforts of F-gases use simplified chemical schemes and ignore three-dimensional dynamics, which limits the quantification of their chemical impacts, and a full suite of F-gases is not currently included in atmospheric chemical transport models. Here, we develop and implement a chemistry module in the GEOS-Chem model with 27 additional F-gases (including minor CFCs, minor HCFCs, HFCs, PFCs, SF<sub>6</sub>, NF<sub>3</sub>, and SO<sub>2</sub>F<sub>2</sub>) with constrained emissions. The updated simulations capture most of the surface mole fraction baseline trends and some pollution events for F-gases in 2020–2021, with a normalized mean bias between −14 % and 5 % at the Mace Head station and −17 % and 3 % at the ShangDianZi station. The impact of emission spatial distributions decreases with lifetime, suggesting that accurate global modeling of the background of long-lived species (>10 years) is less dependent on the spatial distribution of the emission than on the total magnitude. The impact of the updated simulation on key reactive species, including ozone, HO<sub><em>x</em></sub>, ClO<sub><em>x</em></sub>, and NO<sub><em>x</em></sub>, is <1 %. For species with 10-year lifetimes, F-gas chemical losses drive 20–40 % changes in their mixing ratios. 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Developing the chemistry module for 27 fluorinated greenhouse gases (F-gases): Reactions, emissions, and implementation in GEOS-Chem
Fluorinated greenhouse gases (F-gases) are widely used in refrigeration, air-conditioning, semiconductor, and other industries, contributing a total direct radiative forcing only surpassed by carbon dioxide and methane. Current modeling efforts of F-gases use simplified chemical schemes and ignore three-dimensional dynamics, which limits the quantification of their chemical impacts, and a full suite of F-gases is not currently included in atmospheric chemical transport models. Here, we develop and implement a chemistry module in the GEOS-Chem model with 27 additional F-gases (including minor CFCs, minor HCFCs, HFCs, PFCs, SF6, NF3, and SO2F2) with constrained emissions. The updated simulations capture most of the surface mole fraction baseline trends and some pollution events for F-gases in 2020–2021, with a normalized mean bias between −14 % and 5 % at the Mace Head station and −17 % and 3 % at the ShangDianZi station. The impact of emission spatial distributions decreases with lifetime, suggesting that accurate global modeling of the background of long-lived species (>10 years) is less dependent on the spatial distribution of the emission than on the total magnitude. The impact of the updated simulation on key reactive species, including ozone, HOx, ClOx, and NOx, is <1 %. For species with 10-year lifetimes, F-gas chemical losses drive 20–40 % changes in their mixing ratios. Our work provides a comprehensive F-gases chemistry module complementing the major CFCs and HCFCs in the GEOS-Chem model, and this suite of F-gases provides potential applications for understanding their climate impacts and atmospheric processes.
期刊介绍:
Atmospheric Environment has an open access mirror journal Atmospheric Environment: X, sharing the same aims and scope, editorial team, submission system and rigorous peer review.
Atmospheric Environment is the international journal for scientists in different disciplines related to atmospheric composition and its impacts. The journal publishes scientific articles with atmospheric relevance of emissions and depositions of gaseous and particulate compounds, chemical processes and physical effects in the atmosphere, as well as impacts of the changing atmospheric composition on human health, air quality, climate change, and ecosystems.