Detection of Fossil and Biogenic Methane at Regional Scales Using Atmospheric Radiocarbon

Detection of Fossil and Biogenic Methane at Regional Scales Using Atmospheric Radiocarbon
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DOI:
10.1029/2018ef001064
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发表时间:
2019-03-01
期刊:
影响因子:
8.2
通讯作者:
Zazzeri, G.
Zazzeri, G.
中科院分区:
地球科学1区
文献类型:
--
作者:
Graven, H.;Hocking, T.;Zazzeri, G.

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区域甲烷排放量及其归因于各种来源目前存在很大的不确定性。测量甲烷(CH 4)中的放射性碳(C-14)可以提供一种方法,用于识别来自化石源和生物源的区域CH 4排放,因为添加不含C-14的化石碳比生物源碳更能降低大气CH 4中的C-14/C比率(Delta(CH 4)-C-14)。我们描述了一种方法,估计化石和生物甲烷在区域尺度上使用大气三角洲(CH 4)-C-14观测。作为一个案例研究,以证明预期的德尔塔(CH 4)-C-14和德尔塔(CH 4)-C-14-CH 4的关系,我们模拟和比较德尔塔(CH 4)-C-14在加州的网站网络使用两个网格CH 4排放量估计(全球大气研究排放数据库,埃德加和网格环境保护局,GEPA)和2014年的CarbonTracker-Lagrange模型,以及2030年的“一切照旧”和减缓设想方案。CH 4(F)的化石部分与模拟的Delta(CH 4)-C14-CH 4斜率密切相关,2014年埃德加与GEPA的F中值差异为2-21%,2030年照常和减缓情景的差异为7-10%。对于>200 ppb的添加的CH 4,F的差异为10%,产生Delta(CH 4)-C-14的差异>10,这可能从常规观测中检测到。核电厂(CH 4)-C-14排放量通常对Delta(CH 4)-C-14(0-7)的模拟中值影响较小,但在某些大气条件下,它们可能更强(>30),这表明在加州应用Delta(CH 4)-C-14时必须考虑它们。这项研究表明,大气Delta(CH 4)-C-14测量可以对区域CH 4排放量提供强有力的限制,补充其他监测技术。
Regional emissions of methane and their attribution to a variety of sources presently have large uncertainties. Measurements of radiocarbon (C-14) in methane (CH4) may provide a method for identifying regional CH4 emissions from fossil versus biogenic sources because adding C-14-free fossil carbon reduces the C-14/C ratio (Delta(CH4)-C-14) in atmospheric CH4 much more than biogenic carbon does. We describe an approach for estimating fossil and biogenic CH4 at regional scales using atmospheric Delta(CH4)-C-14 observations. As a case study to demonstrate expected Delta(CH4)-C-14 and Delta(CH4)-C-14-CH4 relationships, we simulate and compare Delta(CH4)-C-14 at a network of sites in California using two gridded CH4 emissions estimates (Emissions Database for Global Atmospheric Research, EDGAR, and Gridded Environmental Protection Agency, GEPA) and the CarbonTracker-Lagrange model for 2014, and for 2030 under business-as-usual and mitigation scenarios. The fossil fraction of CH4 (F) is closely linked with the simulated Delta(CH4)-C-14-CH4 slope and differences of 2-21% in median F are found for EDGAR versus GEPA in 2014, and 7-10% for business-as-usual and mitigation scenarios in 2030. Differences of 10% in F for >200 ppb of added CH4 produce differences of >10 in Delta(CH4)-C-14, which are likely detectable from regular observations. Nuclear power plant (CH4)-C-14 emissions generally have small simulated median influences on Delta(CH4)-C-14 (0-7), but under certain atmospheric conditions they can be much stronger (>30) suggesting they must be considered in applications of Delta(CH4)-C-14 in California. This study suggests that atmospheric Delta(CH4)-C-14 measurements could provide powerful constraints on regional CH4 emissions, complementary to other monitoring techniques.