GSTDTAP  > 地球科学
DOI10.5194/acp-20-8405-2020
Strong sensitivity of the isotopic composition of methane to the plausible range of tropospheric chlorine
Strode, Sarah A.1,2; Wang, James S.1,2,6; Manyin, Michael2,3; Duncan, Bryan2; Hossaini, Ryan4; Keller, Christoph A.1,2; Michel, Sylvia E.5; White, James W. C.5
2020-07-17
发表期刊ATMOSPHERIC CHEMISTRY AND PHYSICS
ISSN1680-7316
EISSN1680-7324
出版年2020
卷号20期号:14页码:8405-8419
文章类型Article
语种英语
国家USA; England; Germany
英文摘要

The C-13 isotopic ratio of methane, delta C-13 of CH4, provides additional constraints on the CH4 budget to complement the constraints from CH4 observations. The interpretation of delta C-13 observations is complicated, however, by uncertainties in the methane sink. The reaction of CH4 with Cl is highly fractionating, increasing the relative abundance of (CH4)-C-13, but there is currently no consensus on the strength of the tropospheric Cl sink. Global model simulations of halogen chemistry differ strongly from one another in terms of both the magnitude of tropospheric Cl and its geographic distribution. This study explores the impact of the intermodel diversity in Cl fields on the simulated delta C-13 of CH4. We use a set of GEOS global model simulations with different predicted Cl fields to test the sensitivity of the delta C-13 of CH4 to the diversity of Cl output from chemical transport models. We find that delta C-13 is highly sensitive to both the amount and geographic distribution of Cl. Simulations with Cl providing 0.28 % or 0.66 % of the total CH4 loss bracket the delta C-13 observations for a fixed set of emissions. Thus, even when Cl provides only a small fraction of the total CH4 loss and has a small impact on total CH4, it provides a strong lever on delta C-13. Consequently, it is possible to achieve a good representation of total CH4 using widely different Cl concentrations, but the partitioning of the CH4 loss between the OH and Cl reactions leads to strong differences in isotopic composition depending on which model's Cl field is used. Comparing multiple simulations, we find that altering the tropospheric Cl field leads to approximately a 0.5 parts per thousand increase in delta(CH4)-C-13 for each percent increase in how much CH4 is oxidized by Cl. The geographic distribution and seasonal cycle of Cl also impacts the hemispheric gradient and seasonal cycle of delta C-13. The large effect of Cl on delta C-13 compared to total CH4 broadens the range of CH4 source mixtures that can be reconciled with delta C-13 observations. Stronger constraints on tropospheric Cl are necessary to improve estimates of CH4 sources from delta C-13 observations.


领域地球科学
收录类别SCI-E
WOS记录号WOS:000551526700005
WOS关键词ATMOSPHERIC METHANE ; FOSSIL-FUEL ; CHEMISTRY MODULE ; GROWTH-RATE ; MODEL ; CH4 ; TRANSPORT ; EMISSIONS ; CARBON ; RATIOS
WOS类目Environmental Sciences ; Meteorology & Atmospheric Sciences
WOS研究方向Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences
URL查看原文
引用统计
文献类型期刊论文
条目标识符http://119.78.100.173/C666/handle/2XK7JSWQ/284143
专题地球科学
作者单位1.Univ Space Res Assoc, Columbia, MD 21046 USA;
2.NASA, Goddard Space Flight Ctr, Greenbelt, MD 20771 USA;
3.Sci Syst & Applicat Inc SSAI, Lanham, MD USA;
4.Univ Lancaster, Lancaster Environm Ctr, Lancaster, England;
5.Univ Colorado, Inst Arctic & Alpine Res, Boulder, CO 80309 USA;
6.Inst Adv Sustainabil Studies, Potsdam, Germany
推荐引用方式
GB/T 7714
Strode, Sarah A.,Wang, James S.,Manyin, Michael,et al. Strong sensitivity of the isotopic composition of methane to the plausible range of tropospheric chlorine[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2020,20(14):8405-8419.
APA Strode, Sarah A..,Wang, James S..,Manyin, Michael.,Duncan, Bryan.,Hossaini, Ryan.,...&White, James W. C..(2020).Strong sensitivity of the isotopic composition of methane to the plausible range of tropospheric chlorine.ATMOSPHERIC CHEMISTRY AND PHYSICS,20(14),8405-8419.
MLA Strode, Sarah A.,et al."Strong sensitivity of the isotopic composition of methane to the plausible range of tropospheric chlorine".ATMOSPHERIC CHEMISTRY AND PHYSICS 20.14(2020):8405-8419.
条目包含的文件
条目无相关文件。
个性服务
推荐该条目
保存到收藏夹
查看访问统计
导出为Endnote文件
谷歌学术
谷歌学术中相似的文章
[Strode, Sarah A.]的文章
[Wang, James S.]的文章
[Manyin, Michael]的文章
百度学术
百度学术中相似的文章
[Strode, Sarah A.]的文章
[Wang, James S.]的文章
[Manyin, Michael]的文章
必应学术
必应学术中相似的文章
[Strode, Sarah A.]的文章
[Wang, James S.]的文章
[Manyin, Michael]的文章
相关权益政策
暂无数据
收藏/分享
所有评论 (0)
暂无评论
 

除非特别说明,本系统中所有内容都受版权保护,并保留所有权利。