Emerging investigator series: spatially and temporally resolved lightning NOx production rates obtained with space-based lightning detectors.

IF 4.2 3区 环境科学与生态学 Q1 CHEMISTRY, ANALYTICAL
Rebekah P Horner, Eloise A Marais, Lee T Murray
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引用次数: 0

Abstract

Lightning is a dominant free tropospheric source of nitrogen oxides (NOx), impacting climate by affecting global tropospheric ozone (O3) and other key oxidants. We calculate temporally and spatially resolved lightning NOx (LNOx) production rates using lightning flash energies from space-based Lightning Imaging Sensors (LIS). Our production rates average ∼309 moles per flash (mol fl-1) over oceans, peaking at midday, and ∼172 mol fl-1 over land, peaking in the early morning. Replacing static values in the original GEOS-Chem model inventory with our spatially and hourly varying production rates yields global annual LNOx emissions of 4.4 Tg nitrogen (N) for 2015-2019; almost 2 Tg N less than the original inventory. Annual terrestrial LNOx emissions still exceed those over the ocean, due to more frequent lightning over land, but the relative proportion of maritime emissions increases. The largest decline in LNOx emissions is north of 35°N in summer, as static 500 mol fl-1 is replaced with 150-250 mol fl-1. Global decline in LNOx emissions decreases abundances of free tropospheric NOx, O3, the hydroxyl radical (OH) and peroxyacetyl nitrate (PAN). Hourly variability in LIS flash radiances is broadly consistent with high-frequency Geostationary Lightning Mapper (GLM) flash energies, though the comparison is limited to tropical America. Introducing hourly variability in LNOx production rates leads to a greater than 10% localised decline in equatorial lower tropospheric O3. Independent validation is critically needed, given our updated LNOx emissions offer a viable solution to model overestimates in O3 and OH and underestimates in the lifetime of the greenhouse gas methane.

新兴研究者系列:空间和时间解决闪电氮氧化物产生率获得天基闪电探测器。
闪电是氮氧化物(NOx)的主要自由对流层来源,通过影响全球对流层臭氧(O3)和其他主要氧化剂来影响气候。我们利用天基闪电成像传感器(LIS)的闪电能量计算了时间和空间分辨的闪电NOx (LNOx)产生率。我们的生产速度平均为每闪~ 309摩尔(mol fl-1),在海洋上空达到峰值,在中午达到峰值,在陆地上达到峰值,在清晨达到峰值。将原始GEOS-Chem模型库存中的静态值替换为我们的空间和小时变化生产率,2015-2019年全球年LNOx排放量为4.4 Tg氮(N);几乎比原始库存少了2tg N。由于陆地上的闪电更加频繁,陆地每年的LNOx排放量仍然超过海洋,但海洋排放的相对比例有所增加。夏季LNOx排放量下降幅度最大的是在35°N以北,静态的500 mol fl-1被150-250 mol fl-1所取代。全球LNOx排放的减少降低了对流层中游离NOx、O3、羟基自由基(OH)和过氧乙酰硝酸盐(PAN)的丰度。LIS闪光辐射的每小时变化与高频地球静止闪电绘图仪(GLM)闪光能量大致一致,尽管比较仅限于热带美洲。引入LNOx生成速率的小时变率导致赤道对流层低层O3局地下降超过10%。考虑到我们最新的LNOx排放为模型中O3和OH的高估以及温室气体甲烷生命周期的低估提供了可行的解决方案,因此独立验证是非常必要的。
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来源期刊
Environmental Science: Processes & Impacts
Environmental Science: Processes & Impacts CHEMISTRY, ANALYTICAL-ENVIRONMENTAL SCIENCES
CiteScore
9.50
自引率
3.60%
发文量
202
审稿时长
1 months
期刊介绍: Environmental Science: Processes & Impacts publishes high quality papers in all areas of the environmental chemical sciences, including chemistry of the air, water, soil and sediment. We welcome studies on the environmental fate and effects of anthropogenic and naturally occurring contaminants, both chemical and microbiological, as well as related natural element cycling processes.
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