SDU-C多相化学大气模拟室─甲基乙二醛SOA的初步研究

IF 2.6 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY ACS Earth and Space Chemistry Pub Date : 2026-10-15 Epub Date: 2026-09-15 DOI:10.1021/acsearthspacechem.6c00209
Mujahid Ali, Hui Tian, Yanhao Wei, Lin He, Liang Wen, Majda Mekic, Thomas Schaefer, Shuguang Wang, Xiaomin Sun, Min Song, Jinhe Wang, Yimu Zhang, Likun Xue, Lin Du, Yang Zeng, Christian George, Abdelwahid Mellouki, Jianmin Chen, Hartmut Herrmann
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After introducing the facility\r\nand its characteristics, the effects of initial methylglyoxal (MGLY)\r\nconcentration, seed acidity, and relative humidity (RH) on secondary\r\norganic aerosol (SOA) formation from MGLY photooxidation in a coupled\r\ngas–particle system are examined. The Shandong University atmospheric\r\nsimulation chamber (SDU-C), located on Qingdao Campus, China, is a\r\nfully computer-controlled, collapsible 18 m<sup>3</sup> cylindrical\r\nchamber made of a 0.7 mm thick Teflon film, with a diameter of 3 m\r\nand a height of 2.4 m. Characterization experiments determined the\r\nSDU-C light intensity and wall-loss rates of NO<sub>2</sub>, NO, O<sub>3</sub>, and seed particles. The NO<sub>2</sub> photolysis frequency,\r\nJ(NO<sub>2</sub>), was (4.5 ± 0.02) ×10<sup>–4</sup>·s<sup>–1</sup>, while the wall-loss rates for NO, NO<sub>2</sub>, O<sub>3</sub>, and seed particles were (1.6 ± 0.1)\r\n×10<sup>–6</sup>·s<sup>–1</sup>, (6.6 ±\r\n1.4) ×10<sup>–6</sup>·s<sup>–1</sup>, (4.2\r\n± 0.7) ×10<sup>–6</sup>·s<sup>–1</sup>, and (4.4 ± 0.4) ×10<sup>–5</sup>·s<sup>–1</sup>, respectively. As its first application, a series of MGLY photooxidation\r\nexperiments were conducted with gas-phase oxidation initiated by OH\r\nradicals. Results showed that the initial MGLY uptake and photooxidation-driven\r\nSOA formation increased with higher initial MGLY concentration [MGLY]<sub>0</sub>, seed acidity, and RH. At 11% RH with neutral seeds, particle\r\nmass increased from 0.4 to 26.9 and 31.4 μg·m<sup>–3</sup> as the initial MGLY concentration increased from 72 to 144 and 216\r\nppb, respectively. 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引用次数: 0

摘要

大气模拟室是在接近真实条件下研究大气过程的可控实验平台。本文介绍了一种专门用于对流层多相化学研究的新设备。在介绍了该装置及其特点后,研究了初始甲基乙二醛(MGLY)浓度、种子酸度和相对湿度(RH)对MGLY光氧化在耦合气-粒子系统中形成二次有机气溶胶(SOA)的影响。山东大学大气模拟室(SDU-C)位于中国青岛校区,是一个完全由计算机控制的可折叠18立方米的圆柱形室,由0.7毫米厚的聚四氟乙烯薄膜制成,直径为3,高度为2.4米。表征实验确定了sdu - c的光强和NO2、NO、O3和种子颗粒的壁损率。NO2光解频率J(NO2)为(4.5±0.02)×10-4·s-1,而NO、NO2、O3和种子颗粒的壁损率分别为(1.6±0.1)×10-6·s-1、(6.6±1.4)×10-6·s-1、(4.2±0.7)×10-6·s-1和(4.4±0.4)×10-5·s-1。作为其首次应用,我们进行了一系列由氧自由基引发气相氧化的MGLY光氧化实验。结果表明,随着初始MGLY浓度[MGLY]0、种子酸度和相对湿度的增加,MGLY的初始吸收和光氧化驱动的soa形成增加。在11% RH条件下,中性种子的初始MGLY浓度分别从72增加到144和216ppb,颗粒质量分别从0.4增加到26.9和31.4 μg·m-3。紫外线A (UVA)照射后,在50% RH和216 ppb MGLY条件下,超酸性种子的SOA质量达到43.2 μg·m-3。大多数颗粒相MGLY存在低聚物(>95%),具有较高的[MGLY]0和RH,而强酸性使单体水平升高。总体而言,表征结果和首次应用表明,SDU-C为探索受控条件下的大气多相化学、气-颗粒划分和SOA形成提供了可靠的实验平台。
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The SDU-C Atmospheric Simulation Chamber for Multiphase Chemistry─An Initial Study on Methylglyoxal SOA

Atmospheric simulation chambers are controlled experimental platforms used for studying atmospheric processes under near-realistic conditions. Here, a new facility specifically designed for research on tropospheric multiphase chemistry is presented. After introducing the facility and its characteristics, the effects of initial methylglyoxal (MGLY) concentration, seed acidity, and relative humidity (RH) on secondary organic aerosol (SOA) formation from MGLY photooxidation in a coupled gas–particle system are examined. The Shandong University atmospheric simulation chamber (SDU-C), located on Qingdao Campus, China, is a fully computer-controlled, collapsible 18 m3 cylindrical chamber made of a 0.7 mm thick Teflon film, with a diameter of 3 m and a height of 2.4 m. Characterization experiments determined the SDU-C light intensity and wall-loss rates of NO2, NO, O3, and seed particles. The NO2 photolysis frequency, J(NO2), was (4.5 ± 0.02) ×10–4·s–1, while the wall-loss rates for NO, NO2, O3, and seed particles were (1.6 ± 0.1) ×10–6·s–1, (6.6 ± 1.4) ×10–6·s–1, (4.2 ± 0.7) ×10–6·s–1, and (4.4 ± 0.4) ×10–5·s–1, respectively. As its first application, a series of MGLY photooxidation experiments were conducted with gas-phase oxidation initiated by OH radicals. Results showed that the initial MGLY uptake and photooxidation-driven SOA formation increased with higher initial MGLY concentration [MGLY]0, seed acidity, and RH. At 11% RH with neutral seeds, particle mass increased from 0.4 to 26.9 and 31.4 μg·m–3 as the initial MGLY concentration increased from 72 to 144 and 216 ppb, respectively. After ultraviolet A (UVA) irradiation, SOA mass reached 43.2 μg·m–3 for super acidic seeds at 50% RH and 216 ppb MGLY. Most particle-phase MGLY exists as oligomers (>95%), with higher [MGLY]0 and RH, while strong acidity raises monomer levels. Overall, the characterization findings and first application indicate that SDU-C offers a reliable experimental platform for exploring atmospheric multiphase chemistry, gas–particle partitioning, and SOA formation under controlled conditions.

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ACS Earth and Space Chemistry
ACS Earth and Space Chemistry Earth and Planetary Sciences-Geochemistry and Petrology
CiteScore
5.30
自引率
11.80%
发文量
249
期刊介绍: The scope of ACS Earth and Space Chemistry includes the application of analytical, experimental and theoretical chemistry to investigate research questions relevant to the Earth and Space. The journal encompasses the highly interdisciplinary nature of research in this area, while emphasizing chemistry and chemical research tools as the unifying theme. The journal publishes broadly in the domains of high- and low-temperature geochemistry, atmospheric chemistry, marine chemistry, planetary chemistry, astrochemistry, and analytical geochemistry. ACS Earth and Space Chemistry publishes Articles, Letters, Reviews, and Features to provide flexible formats to readily communicate all aspects of research in these fields.
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Issue Editorial Masthead Issue Publication Information A High-Resolution Rotational Analysis of 2-Chloroethanol (HOCH2CH2Cl) and Its First Vibrationally Excited State Mineralogical Heterogeneity Controls Dissolution-Front Instability and Reactive-Transport Scaling in Porous Media The SDU-C Atmospheric Simulation Chamber for Multiphase Chemistry─An Initial Study on Methylglyoxal SOA
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