Multiphase Reactive Bromine Chemistry during Late Spring in the Arctic: Measurements of Gases, Particles, and Snow
Multiphase Reactive Bromine Chemistry during Late Spring in the Arctic: Measurements of Gases, Particles, and Snow
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北极晚春期间的多相活性溴化学：气体、颗粒和雪的测量
DOI：
10.1021/acsearthspacechem.2c00189
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发表时间：
2022
影响因子：
3.4
通讯作者：
Shepson, Paul B.
中科院分区：
文献类型：
--
作者：
Jeong, Daun;McNamara, Stephen M.;Barget, Anna J.;Raso, Angela R.;Upchurch, Lucia M.;Thanekar, Sham;Quinn, Patricia K.;Simpson, William R.;Fuentes, Jose D.;Shepson, Paul B.
在极地日出后，溴自由基会导致北极大气边界层中的臭氧消耗和汞沉积。这些溴自由基主要是由分子溴(Br2)的光解形成的，而溴分子是在积雪中以光化学方式产生的。最近的研究表明，在北极春季末期融雪之前，溴与臭氧反应生成的溴一氧化二氮(Bro·)一直存在。为了检查这次反应溴化学倒春关闭的驱动因素，在春季(2016年3月至5月)期间，在阿拉斯加乌特卡格̇vik附近使用化学电离质谱仪连续监测了Br2、HOBr3、BrO和BrCl4种气体。5月10日，在气温上升到0°C以上，地表反照率降低，并观察到积雪开始融化的同时，所有四种活性溴物种都低于检测水平。在大气溴化学停止之前，5月初的当地地表雪样变得显著富含溴，这可能是由于反应性溴循环的放缓，继续沉积，但减少了积雪的排放。颗粒溴浓度不足以解释在积雪融化时观察到的和减少的反应性溴气体的数量。在活性溴化学停止前几周的低风速表明，吹雪对溴化学没有贡献。总而言之，这些结果进一步突出了地表积雪在多阶段溴再循环中的重要性，并具有重要意义，因为由于气候变化，融化季节提前到来。
Bromine radicals (Br·) cause ozone depletion and mercury deposition in the Arctic atmospheric boundary layer, following Polar sunrise. These Br radicals are primarily formed by the photolysis of molecular bromine (Br2), which is photochemically produced in the snowpack. Recently, it was shown that bromine monoxide (BrO·), formed from the reaction of Br· with ozone, is episodically present until the onset of snowmelt in late Arctic spring. To examine the drivers of this late spring shutdown of reactive bromine chemistry, the gases Br2, HOBr, BrO, and BrCl were continuously monitored using chemical ionization mass spectrometry during the spring (March–May 2016) near Utqiaġvik, Alaska. On May 10th, all four reactive bromine species fell below levels of detection at the same time that air temperature increased above 0 °C, surface albedo decreased, and snowmelt onset was observed. Prior to the cessation of atmospheric bromine chemistry, local surface snow samples in early May became significantly enriched in bromide, likely due to the slowdown of reactive bromine recycling with continued deposition but decreased emissions from the snowpack. Particulate bromide concentrations were not sufficient to explain the quantities of reactive bromine gases observed and decreased upon snowmelt. Low wind speeds during the weeks preceding the cessation of reactive bromine chemistry point to the lack of a contribution to bromine chemistry from blowing snow. Together, these results further highlight the significance of the surface snowpack in multiphase bromine recycling with important implications as the melt season arrives earlier due to climate change.
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作者：
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影响因子：
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作者：
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DOI：
--
发表时间：
1994
期刊：
影响因子：
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作者：
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