Aqueous secondary organic aerosol formation from the direct photosensitized oxidation of vanillin in the absence and presence of ammonium nitrate

Aqueous secondary organic aerosol formation from the direct photosensitized oxidation of vanillin in the absence and presence of ammonium nitrate
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在不存在和存在硝酸铵的情况下,香草醛直接光敏氧化形成水性二次有机气溶胶

DOI:
10.5194/acp-22-273-2022
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发表时间:
2022-01
影响因子:
6.3
通讯作者:
Chak K. Chan
Chak K. Chan
中科院分区:
地球科学1区
文献类型:
--
作者:
Beatrix Rosette Go Mabato;Yan Lyu;Yan Ji;Yong Jie Li;Dan Dan Huang;Xue Li;Theodora Nah;Chun Ho Lam;Chak K. Chan

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抽象的。香草醛(VL)是生物质燃烧排放物中丰富的酚类芳族羰基化合物,在模拟阳光下形成三重激发态(3VL π),导致水性二次有机气溶胶(aqSOA)形成。硝酸盐和铵是生物质、燃烧气溶胶和云水或雾水的主要成分。在大气相关的云和雾的条件下,溶液组成的VL只有或VL与硝酸铵进行模拟阳光照射,比较aqSOA的形成通过直接光敏氧化的VL在硝酸铵的存在和不存在。通过检查VL衰减动力学、产物组成和吸光度变化来表征反应。这两种条件下产生的低聚物,官能化单体,和含氧开环产品,硝酸铵促进功能化和硝化,可能是由于其光解产物(OH,NO2,NO2-或HONO)。此外,在硝酸铵存在下观察到的潜在咪唑衍生物表明铵参与了反应。大多数最丰富的产品从这两种条件下的潜在的棕色碳(BrC)发色团。氧气(O2),pH值,反应物的浓度和摩尔比对反应的影响进行了探讨。我们的研究结果表明,O2在反应中起着至关重要的作用,并且在pH值下,寡聚物的形成得到增强
Abstract. Vanillin (VL), a phenolic aromatic carbonyl abundant in biomass burning emissions, forms triplet excited states (3VL∗) under.simulated sunlight leading to aqueous secondary organic aerosol (aqSOA).formation. Nitrate and ammonium are among the main components of biomass.burning aerosols and cloud or fog water. Under atmospherically relevant cloud and fog conditions, solutions composed of either VL only or VL with ammonium nitrate were subjected to simulated sunlight irradiation to compare aqSOA formation via the direct photosensitized oxidation of VL in the absence and presence of ammonium nitrate. The reactions were characterized by examining the VL decay kinetics, product compositions, and light absorbance changes. Both conditions generated oligomers, functionalized monomers, and oxygenated ring-opening products, and ammonium nitrate promoted functionalization and nitration, likely due to its photolysis products (⚫OH, ⚫NO2, and NO2- or HONO). Moreover, a potential imidazole derivative observed in the presence of ammonium nitrate suggested that ammonium participated in the reactions. The majority of the most abundant products from both conditions were potential brown carbon (BrC) chromophores. The effects of oxygen (O2), pH, and reactants concentration and molar ratios on the reactions were also explored. Our findings show that O2 plays an essential role in the reactions, and oligomer formation was enhanced at pH
秋季,中国中部城市上空生物质燃烧加剧,成为气溶胶铵的来源
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