全面评估温度升高对灯管封闭式氧化流动反应器(OFR)系统中气体和气溶胶化学性质的影响

IF 3.2 3区 地球科学 Q2 METEOROLOGY & ATMOSPHERIC SCIENCES Atmospheric Measurement Techniques Pub Date : 2024-08-27 DOI:10.5194/amt-17-4915-2024
Tianle Pan, Andrew T. Lambe, Weiwei Hu, Yicong He, Minghao Hu, Huaishan Zhou, Xinming Wang, Qingqing Hu, Hui Chen, Yue Zhao, Yuanlong Huang, Doug R. Worsnop, Zhe Peng, Melissa A. Morris, Douglas A. Day, Pedro Campuzano-Jost, Jose-Luis Jimenez, Shantanu H. Jathar
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引用次数: 0

摘要

摘要。氧化流动反应器(OFR)已被广泛用于研究二次有机气溶胶(SOA)的形成。然而,如果不对紫外灯的影响进行彻底评估,通常用于启动氧化流动反应器中的光化学反应的紫外灯可能会导致反应器温度升高。在这项研究中,我们对 Aerodyne 潜在气溶胶质量 OFR(PAM-OFR)内的温度分布进行了全面调查,然后研究了灯管加热对流动和化学反应的后续影响。我们观察到了灯管引起的温度升高,这与灯管驱动电压、灯管数量、灯管类型、OFR停留时间以及PAM-OFR内的位置有关。在典型的 PAM-OFR 运行条件下(例如,在低氮氧化物条件下,小于 5 d 的等效大气 OH 暴露),温度通常会升高 1-5 °C。在极端条件下(但较少出现),升温可高达 15 °C。我们评估了与环境条件相比温度升高对 PAM-OFR 内部的流量分布、气体和凝聚相化学的影响。我们的研究结果表明,温度的升高改变了流场,导致停留时间分布和相应的氧化剂暴露尾迹减少,原因是再循环速度加快。根据自由基化学箱模型的模拟结果,温度升高对 PAM-OFR 内氧化剂绝对浓度的影响极小(< 5%)。此外,还研究了温度对种子有机气溶胶(OA)和新形成的二次有机气溶胶的影响,结果表明,温度升高会影响具有代表性的生物和人为 SOA 类型的产量、大小和氧化水平。我们提出了与温度相关的 SOA 产量修正建议和 PAM-OFR 操作规程,以减轻灯管引起的温度升高和波动。我们建议在 PAM-OFR 实验期间用风扇在反应器外部吹风,以尽量减少 PAM-OFR 内的温度升高。与 Aerodyne 版本相比,使用功率较小的灯管的 OFR 的温度升幅要低得多。
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A comprehensive evaluation of enhanced temperature influence on gas and aerosol chemistry in the lamp-enclosed oxidation flow reactor (OFR) system
Abstract. Oxidation flow reactors (OFRs) have been extensively utilized to examine the formation of secondary organic aerosol (SOA). However, the UV lamps typically employed to initiate the photochemistry in OFRs can result in an elevated reactor temperature when their implications are not thoroughly evaluated. In this study, we conducted a comprehensive investigation into the temperature distribution within an Aerodyne potential aerosol mass OFR (PAM-OFR) and then examined the subsequent effects on flow and chemistry due to lamp heating. A lamp-induced temperature increase was observed, which was a function of lamp-driving voltage, number of lamps, lamp types, OFR residence time, and positions within the PAM-OFR. Under typical PAM-OFR operational conditions (e.g., < 5 d of equivalent atmospheric OH exposure under low-NOx conditions), the temperature increase typically ranged from 1–5 °C. Under extreme (but less frequently encountered) conditions, the heating could reach up to 15 °C. The influences of the increased temperature over ambient conditions on the flow distribution, gas, and condensed-phase chemistry within PAM-OFR were evaluated. Our findings indicate that the increase in temperature altered the flow field, resulting in a diminished tail on the residence time distribution and corresponding oxidant exposure due to faster recirculation. According to simulation results from a radical chemistry box model, the variation in absolute oxidant concentration within PAM-OFR due to temperature increase was minimal (< 5 %). The temperature influences on seed organic aerosol (OA) and newly formed secondary OA were also investigated, suggesting that an increase in temperature can impact the yield, size, and oxidation levels of representative biogenic and anthropogenic SOA types. Recommendations for temperature-dependent SOA yield corrections and PAM-OFR operating protocols that mitigate lamp-induced temperature enhancement and fluctuations are presented. We recommend blowing air around the reactor's exterior with fans during PAM-OFR experiments to minimize the temperature increase within PAM-OFR. Temperature increases are substantially lower for OFRs utilizing less powerful lamps compared to the Aerodyne version.
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来源期刊
Atmospheric Measurement Techniques
Atmospheric Measurement Techniques METEOROLOGY & ATMOSPHERIC SCIENCES-
CiteScore
7.10
自引率
18.40%
发文量
331
审稿时长
3 months
期刊介绍: Atmospheric Measurement Techniques (AMT) is an international scientific journal dedicated to the publication and discussion of advances in remote sensing, in-situ and laboratory measurement techniques for the constituents and properties of the Earth’s atmosphere. The main subject areas comprise the development, intercomparison and validation of measurement instruments and techniques of data processing and information retrieval for gases, aerosols, and clouds. The manuscript types considered for peer-reviewed publication are research articles, review articles, and commentaries.
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