Suspect screening for pesticides in rain and snow using liquid chromatography high-resolution mass spectrometry

Suspect screening for pesticides in rain and snow using liquid chromatography high-resolution mass spectrometry
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利用液相色谱高分辨质谱法筛查雨雪中农药疑似物

DOI:
10.1016/j.atmosenv.2022.119389
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发表时间:
2022
影响因子:
5
通讯作者:
Faust, Jennifer A.
Faust, Jennifer A.
中科院分区:
环境科学与生态学2区
文献类型:
--
作者:
Gray, Rebekah;Painter, Eve;Sprankle, Jameson W.;Crawford, Alex D.;Morrison, Jillian J.;Frazier, Marian;Faust, Jennifer A.

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羰基化合物是大气中自由基、臭氧(O3)和二次有机气溶胶(SOA)的重要前体。生物质燃烧是羰基化合物的重要来源。为了探索生物质燃烧中羰基化合物的形成途径以及燃料组成和燃烧条件的影响,本研究在7个点火温度(300-900°C, 100°C梯度)和2个氧气浓度(21%和10.5%)下,使用3种生物质类型(稻草、松树和杨树)及其3种成分提取物(纤维素、半纤维素和木质素)进行了管炉燃烧实验。结果表明:水稻秸秆、松木秸秆和杨木秸秆中羰基化合物(EFCC)的平均排放因子分别为2.28±1.72、3.09±2.98和2.90±2.78 g/kg;低温期(300 ~ 500℃)efcc(5.37±0.25 g/kg)显著高于高温期(0.55±0.03 g/kg)。此外,氧还原促进了羰基化合物的排放,使efcce平均增加21.6%。3种生物质组分的平均efcc依次为纤维素(3.78±3.90 g/kg)、半纤维素(2.90±2.60 g/kg)和木质素(1.98±1.72 g/kg),且cc分布不同。纤维素和半纤维素比木质素产生更多的甲醛和乙醛,分别为71.1±12.6%、69.0±4.4%和62.4±15.5%。丙酮主要由半纤维素和木质素燃烧产生。芳香醛主要由木质素燃烧产生,且受温度影响显著,高温下的比例是低温下的2.7倍。加权平均计算结果表明,3种组分的efcc值与母体燃料的拟合结果较好(r = 0.98),而芳香醛等组分的拟合结果相对较弱(r = 0.66),说明不同组分之间存在不同的形成途径以及对燃料成分和燃烧条件的敏感性。
Carbonyl compounds are important precursors of free radicals, ozone (O3), and secondary organic aerosols (SOA) in the atmosphere. Biomass burning is an important source of carbonyl compounds. To explore the formation pathway of carbonyl compounds from biomass burning and the effects of fuel composition and burning conditions, this study performed tube-furnace combustion experiments using three biomass types (rice straw, pine, and poplar) and their three component extracts (cellulose, hemicellulose, and lignin) at seven ignition temperatures (300–900 °C, 100 °C gradient) and two oxygen concentrations (21% and 10.5%). The results showed that the average emission factors of carbonyl compounds (EFCC) from rice straw, pine, and poplar were 2.28 ± 1.72, 3.09 ± 2.98, and 2.90 ± 2.78 g/kg, respectively. EFCCwere significantly higher (5.37 ± 0.25 g/kg) in lower temperature (300–500 °C) stage than in higher temperature (0.55 ± 0.03 g/kg). Furthermore, oxygen reduction promoted the emission of carbonyl compounds, increasing the EFCCby 21.6% on average. The average EFCCfor the three components of biomass decreased in the order of cellulose (3.78 ± 3.90 g/kg), hemicellulose (2.90 ± 2.60 g/kg) and lignin (1.98 ± 1.72 g/kg), and their CCs profiles were also different. Cellulose and hemicellulose produced more formaldehyde and acetaldehyde than lignin, contributing 71.1 ± 12.6%, 69.0 ± 4.4% and 62.4 ± 15.5% in CCs, respectively. Acetone was mainly produced by the combustion of hemicellulose and lignin. Aromatic aldehydes were mainly produced by lignin burning, and also were significantly affected by temperature, the proportion under higher temperature is 2.7 times that under lower temperature. The EFCCvalues by weighted average calculation from the three components were good matched with those of parent fuels (r = 0.98), while the fitting results for those species such as aromatic aldehydes were relatively weak (r = 0.66), showing that there are different formation pathways and sensitivity to fuel composition and burning condition among different CCs.
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