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Validating HONO as an Intermediate Tracer of the External Cycling of Reactive Nitrogen in the Background Atmosphere
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2023-03-17 , DOI: 10.1021/acs.est.2c06731 Jianshu Wang 1 , Yingjie Zhang 1 , Chong Zhang 1 , Yaru Wang 1 , Jiacheng Zhou 2 , Lisa K Whalley 3 , Eloise J Slater 3 , Joanna E Dyson 3 , Wanyun Xu 4 , Peng Cheng 5 , Baobin Han 5 , Lifan Wang 1 , Xuena Yu 1 , Youfeng Wang 1 , Robert Woodward-Massey 1 , Weili Lin 6 , Weixiong Zhao 2 , Limin Zeng 1 , Zhiqiang Ma 7 , Dwayne E Heard 3 , Chunxiang Ye 1
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2023-03-17 , DOI: 10.1021/acs.est.2c06731 Jianshu Wang 1 , Yingjie Zhang 1 , Chong Zhang 1 , Yaru Wang 1 , Jiacheng Zhou 2 , Lisa K Whalley 3 , Eloise J Slater 3 , Joanna E Dyson 3 , Wanyun Xu 4 , Peng Cheng 5 , Baobin Han 5 , Lifan Wang 1 , Xuena Yu 1 , Youfeng Wang 1 , Robert Woodward-Massey 1 , Weili Lin 6 , Weixiong Zhao 2 , Limin Zeng 1 , Zhiqiang Ma 7 , Dwayne E Heard 3 , Chunxiang Ye 1
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In the urban atmosphere, nitrogen oxide (NOx═NO + NO2)-related reactions dominate the formation of nitrous acid (HONO). Here, we validated an external cycling route of HONO and NOx, i.e., formation of HONO resulting from precursors other than NOx, in the background atmosphere. A chemical budget closure experiment of HONO and NOx was conducted at a background site on the Tibetan Plateau and provided direct evidence of the external cycling. An external daytime HONO source of 100 pptv h–1 was determined. Both soil emissions and photolysis of nitrate on ambient surfaces constituted likely candidate mechanisms characterizing this external source. The external source dominated the chemical production of NOx with HONO as an intermediate tracer. The OH production was doubled as a result of the external cycling. A high HONO/NOx ratio (0.31 ± 0.06) during the daytime was deduced as a sufficient condition for the external cycling. Literature review suggested the prevalence of high HONO/NOx ratios in various background environments, e.g., polar regions, pristine mountains, and forests. Our analysis validates the prevalence of external cycling in general background atmosphere and highlights the promotional role of external cycling regarding the atmospheric oxidative capacity.
中文翻译：
验证 HONO 作为背景大气中活性氮外循环的中间示踪剂
在城市大气中，氮氧化物 (NO x = NO + NO 2 ) 相关反应主导亚硝酸 (HONO) 的形成。在这里，我们验证了 HONO 和 NO x的外部循环路线，即在背景大气中由 NO x以外的前体产生的 HONO 的形成。HONO 和 NO x的化学收支闭合实验在青藏高原的背景地点进行，并提供了外部循环的直接证据。100 pptv h –1的外部日间 HONO 源被确定。土壤排放和环境表面硝酸盐的光解都构成了表征这种外部来源的可能候选机制。外部来源主导了以 HONO 作为中间示踪剂的 NO x的化学生产。由于外部循环，OH 产量翻了一番。白天的高 HONO/NO x比率 (0.31 ± 0.06) 被推断为外部循环的充分条件。文献综述表明高 HONO/NO x的流行各种背景环境中的比率，例如极地地区、原始山脉和森林。我们的分析验证了一般背景大气中外部循环的普遍性，并强调了外部循环对大气氧化能力的促进作用。
更新日期：2023-03-17
中文翻译：
验证 HONO 作为背景大气中活性氮外循环的中间示踪剂
在城市大气中，氮氧化物 (NO x = NO + NO 2 ) 相关反应主导亚硝酸 (HONO) 的形成。在这里，我们验证了 HONO 和 NO x的外部循环路线，即在背景大气中由 NO x以外的前体产生的 HONO 的形成。HONO 和 NO x的化学收支闭合实验在青藏高原的背景地点进行，并提供了外部循环的直接证据。100 pptv h –1的外部日间 HONO 源被确定。土壤排放和环境表面硝酸盐的光解都构成了表征这种外部来源的可能候选机制。外部来源主导了以 HONO 作为中间示踪剂的 NO x的化学生产。由于外部循环，OH 产量翻了一番。白天的高 HONO/NO x比率 (0.31 ± 0.06) 被推断为外部循环的充分条件。文献综述表明高 HONO/NO x的流行各种背景环境中的比率，例如极地地区、原始山脉和森林。我们的分析验证了一般背景大气中外部循环的普遍性，并强调了外部循环对大气氧化能力的促进作用。
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