基于二甘醇的气溶胶粒径谱仪在测量3 nm 以下颗粒物时的性能比较

大气与环境光学学报 ›› 2020, Vol. 15 ›› Issue (6): 470-485.

• “纳米颗粒物在线测量技术”专辑 • 上一篇下一篇

基于二甘醇的气溶胶粒径谱仪在测量3 nm 以下颗粒物时的性能比较

杨栋森1, 蔡润龙2, 蒋靖坤2, 马嫣1, 郑军1∗

1 南京信息工程大学大气环境与装备技术协同创新中心, 江苏南京 210044; 2 清华大学环境学院环境模拟与污染控制国家重点联合实验室, 北京 100084

收稿日期:2020-08-27 修回日期:2020-09-29 出版日期:2020-11-28 发布日期:2020-12-10
通讯作者: E-mail: zheng.jun@nuist.edu.cn E-mail:zheng.jun@nuist.edu.cn
作者简介:杨栋森 (1993- ), 江苏南通人, 博士研究生, 主要从事新粒子生成观测方面的研究。 E-mail: yangdongsen93@163.com
基金资助:
Supported by National Key Research and Development Project (国家重点研发计划, 2017YFC020501), National Natural Science Foundation of China (国家自然科学基金, 91644213, 41730106, 41975172, 41675126)

Performance Intercomparison of Diethylene Glycol-Based Aerosol Size Spectrometers in Sub-3 nm Particle Size Range #br#

YANG Dongsen1, CAI Runlong2, JIANG Jingkun2, MA Yan1, ZHENG Jun1∗ #br#

1 Collaborative Innovation Center of Atmospheric Environment and Equipment Technology, Nanjing University of Information Science & Technology, Nanjing 210044, China; 2 State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China

Received:2020-08-27 Revised:2020-09-29 Published:2020-11-28 Online:2020-12-10
Contact: Jun ZHENG E-mail:zheng.jun@nuist.edu.cn
Supported by:
Supported by National Key Research and Development Project (国家重点研发计划, 2017YFC020501), National Natural Science Foundation of China (国家自然科学基金, 91644213, 41730106, 41975172, 41675126)

摘要/Abstract

摘要： 近年来, 基于二甘醇的气溶胶粒径谱仪被广泛用于 3 nm 以下气溶胶颗粒物的粒径谱测量, 探究比较这些仪器的性能对于粒径谱的准确测量有着重要的意义。对基于二甘醇的扫描电迁移率粒径谱仪 (DEG-SMPS) 和颗粒物粒径放大器 (PSM) 进行了比较研究。在实验室标定过程中, 为让 PSM 获得更可靠的数据, 建议尽可能将标定范围设定至大于 4 nm, 以减少 3 nm 以上的颗粒物在数据反演过程中的影响, 还可以增加 PSM 数据反演的粒径范围。研究表明, PSM 和 DEG-SMPS 在测量小于 3 nm 的颗粒物数浓度时, 结果较为一致。在外场观测的每个新粒子生成天, 这两种仪器之间的数浓度相关性均很好 (r2 >0.75)。但 PSM 与 DEG-SMPS 总数浓度比值的斜率在 1.4 到 4.5 之间变化, 推测可能是由于新粒子生成的颗粒物化学组分的不同导致的。此外, 一些不可忽略的不确定因素, 如两台仪器标定检测效率所产生的不确定度以及 DEG-SMPS 使颗粒物带电时荷电效率的不确定度等, 也可能导致该比对结果的差异。由于 DEG-SMPS 使用静电气溶胶分级器 (DMA) 对颗粒物的粒径进行区分, 而 PSM 是通过改变二甘醇的过饱和度以激活不同粒径的颗粒物, 进而通过数据反演来对粒径进行区分, 因此 DEG-SMPS 的粒径分辨率比 PSM 要高。但 PSM 在低颗粒物数浓度的环境中表现更好, 包括一些较弱的新粒子生成天, 这是因为 PSM 不需要使颗粒物带电, 从而避免了 3 nm 以下颗粒物的极低的荷电效率的问题。因此相比于 DEG-SMPS, PSM 不容易受到凝聚核粒子计数器 (CPC) 的计数误差带来的影响。总的来说, PSM 和 DEG-SMPS 都足以用于测量 3 nm 以下颗粒物的粒径谱分布, 有助于更好地进行新粒子生成过程的研究, 结果中仍然存在的部分不可忽略的不确定性问题需要在未来的研究中进一步解决。

关键词: 气溶胶检测, 粒径谱仪, 粒径谱分布, 新粒子生成

Abstract: Diethylene glycol-based aerosol size spectrometers have been extensively employed to measure sub-3 nm size-resolved particle concentrations in recent years. Quantification of the performance of these instruments for accurate measurement of particle size distribution is essential and significant. Comparison between diethylene glycol-based scanning mobility size spectrometer (DEG-SMPS) and scanning mode particle size magnifier (PSM) was performed. During the laboratory calibrations, to obtain more reliable data by the PSM, the particle size bin larger than 4 nm is recommended to be set during calibration to reduce the influence of large particles during the inversion and increase the inverted size range of the PSM results as well. It is shown that the results of PSM and DEG-SMPS are almost consistent when measuring the number concentration of particles below 3 nm. The correlation of the number concentration between the two instruments in this study is high, with r2 > 0.75 for each day. However, the slope of the total number concentration of PSM versus that of DEG-SMPS varies from 1.4 to 4.5 in this study, which most likely due to the variations in the chemical composition of newly formed particles. In addition, some non-negligible uncertainties, such as the uncertainty caused by the detection efficiency calibration and the uncertainty in the aerosol charge fraction, may also contribute to the difference in the intercomparison. DEG-SMPS classifies particles with DMA and thus can achieve a superior sizing resolution over PSM. Compared with DEG-SMPS, PSM performs better in environment with low particle concentrations, including the days with weak nucleation, due to the fact that PSM completely avoids the low charging efficiency issue of sub-3 nm particles and is less likely affected by the counting uncertainty of a typical CPC in the SMPS system in“magnification stage”. In general, PSM and DEG-SMPS are both adequate for measuring sub-3 nm particle size distributions to better understand new particle formation processes, even some non-negligible uncertainties in the data need to be solved in future research.

Key words: aerosol detection, aerosol size spectrometers, particle size distribution, new particle formation

中图分类号:

X851
P415.3

杨栋森, 蔡润龙, 蒋靖坤, 马嫣, 郑军∗. 基于二甘醇的气溶胶粒径谱仪在测量3 nm 以下颗粒物时的性能比较[J]. 大气与环境光学学报, 2020, 15(6): 470-485.

YANG Dongsen, CAI Runlong, JIANG Jingkun, MA Yan, ZHENG Jun∗. Performance Intercomparison of Diethylene Glycol-Based Aerosol Size Spectrometers in Sub-3 nm Particle Size Range #br# [J]. Journal of Atmospheric and Environmental Optics, 2020, 15(6): 470-485.

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基于二甘醇的气溶胶粒径谱仪在测量3 nm 以下颗粒物时的性能比较

Performance Intercomparison of Diethylene Glycol-Based Aerosol Size Spectrometers in Sub-3 nm Particle Size Range #br#

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