China Meteorological Administration, Institute of Atmospheric Environment, Shenyang, 110166, China.
State Key Laboratory of Severe Weather/Key Laboratory of Atmospheric Chemistry of China Meteorological Administration, Chinese Academy of Meteorological Sciences, Beijing, 100081, China.
Environ Sci Pollut Res Int. 2022 Sep;29(45):67821-67836. doi: 10.1007/s11356-022-20556-9. Epub 2022 May 7.
The formation and evolution of sulfate (SO) and nitrate (NO) secondary contaminants under different stages of pollution episodes and different meteorological and emission conditions were compared, based on the simultaneous observation of fine particulate matter (PM) and its chemical components in four heavy haze pollution episodes at 14 sampling sites in a severe cold climate region of Northeast China in winter from 2017 to 2019. The results yielded two main findings. (1) Nitrate formation during the day was mainly due to the combination of high emissions and high relative humidity (RH, 50-90%), high temperature (T, 0 to 5 °C), high atmospheric oxidizability (ozone (O) and nitrous acid (HONO) concentrations), and high ammonia (NH) concentrations. Nitrate was formed by a gas-phase homogeneous reaction of the hydroxyl radical (OH·) with nitrogen dioxide (NO), sulfur dioxide (SO), and ammonia (NH). (2) The main differences in SO formation between Northeast China and other regions were that the gas-phase oxidation process played an important role. This was mainly a result of the promotion of the gas-phase oxidation of SO due to the high oxidizing ability and the suppression of the aqueous reaction due to the low Ts in winter and low-sulfur coal emissions. Sulfate formation mostly occurred through an aqueous phase reaction in winter, but the highest yield and the fastest production capacity were produced by the gas-phase reaction.
基于 2017 年至 2019 年冬季在中国东北地区严寒气候条件下的 14 个采样点,对 4 次重度雾霾污染过程中细颗粒物(PM)及其化学成分的同步观测,比较了不同污染阶段和不同气象及排放条件下硫酸盐(SO)和硝酸盐(NO)二次污染物的形成和演化。结果得出两个主要结论。(1)白天硝酸盐的形成主要是由于高排放与高相对湿度(50-90%)、高温(0 至 5°C)、高大气氧化性(臭氧(O)和亚硝酸(HONO)浓度)以及高氨(NH)浓度相结合的结果。硝酸盐是由羟基自由基(OH·)与二氧化氮(NO)、二氧化硫(SO)和氨(NH)的气相均相反应形成的。(2)与其他地区相比,中国东北地区 SO 形成的主要差异在于气相氧化过程发挥了重要作用。这主要是由于冬季高氧化能力促进了 SO 的气相氧化,以及低 Ts 和低硫煤排放抑制了水相反应的结果。硫酸盐的形成主要在冬季通过水相反应进行,但气相反应的产率最高,生成速度最快。