Missing Gas-Phase Source of HONO Inferred from Zeppelin Measurements in the Troposphere
Missing Gas-Phase Source of HONO Inferred from Zeppelin Measurements in the Troposphere
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DOI：
10.1126/science.1248999
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发表时间：
2014-04
期刊：
影响因子：
56.9
通讯作者：
Xin Li;F. Rohrer;A. Hofzumahaus;T. Brauers;R. Häseler;B. Bohn;S. Broch;H. Fuchs;S. Gomm;F. Holland;J. Jäger;J. Kaiser;F. Keutsch;I. Lohse;K. Lu;R. Tillmann;R. Wegener;G. Wolfe;T. Mentel;A. Kiendler‐Scharr;A. Wahner
中科院分区：
文献类型：
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作者：
Xin Li;F. Rohrer;A. Hofzumahaus;T. Brauers;R. Häseler;B. Bohn;S. Broch;H. Fuchs;S. Gomm;F. Holland;J. Jäger;J. Kaiser;F. Keutsch;I. Lohse;K. Lu;R. Tillmann;R. Wegener;G. Wolfe;T. Mentel;A. Kiendler‐Scharr;A. Wahner
在齐柏林飞艇上，亚硝酸(HONO)是一种重要的大气痕量气体，它作为对流层羟基自由基(OH)的前体，负责大气的自我净化能力，并控制温室气体的浓度，如甲烷和臭氧。HONO是如何形成的是一个谜。李等人乘坐齐柏林飞艇飞越意大利北部的波谷。(P.292)在未受扰动的早晨对流层中发现了HONO，这表明HONO必须在那里产生，而不是从表面混合。HONO的高浓度很可能是由依赖于光的气相源形成的，它可能消耗了OH或HO2自由基，这表明HONO对整个对流层中OH丰度的影响可能被大大高估了。从依赖光的气相源产生的对流层HONO提出了它对OH的影响的问题。气态亚硝酸(HONO)是对流层羟基自由基(OH)的重要前体。OH负责大气自我净化，并控制甲烷和臭氧等温室气体的浓度。由于缺乏测量，HONO及其来源在对流层中的垂直分布仍然不清楚。在这里，我们呈现了一组关于HONO的观察及其在齐柏林飞艇上所做的预算。在通过温度倒置与地球表面过程分开的阳光照明层中，我们发现高HONO浓度提供了HONO消耗氮氧化物和潜在的氢氧化物的强大气相源的证据。观测到的这一产生过程的性质表明，通常假设的HONO对对流层中OH丰度的影响被大大高估了。
On a Zeppelin Nitrous acid (HONO) is an important atmospheric trace gas that acts as a precursor of tropospheric hydroxyl-radicals (OH), which is responsible for the self-cleansing capacity of the atmosphere and which also controls the concentrations of greenhouse gases, such as methane and ozone. How HONO is made is a mystery. Flying onboard a Zeppelin over the Po Valley in Northern Italy, Li et al. (p. 292) discovered HONO in the undisturbed morning troposphere, indicating that HONO must be produced there, rather than mixed from the surface. The high HONO concentrations are likely to have been formed by a light-dependent gas-phase source that probably consumed OH or HO2 radicals, which hints that the impact of HONO on the abundance of OH in the entire troposphere may be substantially overestimated. The tropospheric production of HONO from a light-dependent gas-phase source raises questions about its impact on OH. Gaseous nitrous acid (HONO) is an important precursor of tropospheric hydroxyl radicals (OH). OH is responsible for atmospheric self-cleansing and controls the concentrations of greenhouse gases like methane and ozone. Due to lack of measurements, vertical distributions of HONO and its sources in the troposphere remain unclear. Here, we present a set of observations of HONO and its budget made onboard a Zeppelin airship. In a sunlit layer separated from Earth’s surface processes by temperature inversion, we found high HONO concentrations providing evidence for a strong gas-phase source of HONO consuming nitrogen oxides and potentially hydrogen oxide radicals. The observed properties of this production process suggest that the generally assumed impact of HONO on the abundance of OH in the troposphere is substantially overestimated.