Jiangkai Ma , Jingjing Meng , Yanhui Wang , Xuan Liu , Xiaoting Zhang , Kaiyue Yang , Qiang Liu , Zhanfang Hou
{"title":"华东聊城草酸同源物的混合状态和演化机制：季节和小时观测的启示","authors":"Jiangkai Ma , Jingjing Meng , Yanhui Wang , Xuan Liu , Xiaoting Zhang , Kaiyue Yang , Qiang Liu , Zhanfang Hou","doi":"10.1016/j.partic.2024.09.011","DOIUrl":null,"url":null,"abstract":"<div><div>Oxalic acid (C<sub>2</sub>) is a significant tracer of secondary organic aerosols (SOA), yet its precursors, evolutionary processes, and formation mechanisms are not fully understood. This knowledge gap leads to uncertainties in evaluating the climate effect and global budget of SOA. Here we compared the size distribution, mixing fraction, and evolutionary mechanism of C<sub>2</sub>-containing particles between summer and winter. In summer, the number of C<sub>2</sub> particles and their homologs decreased compared to winter. However, the proportion of C<sub>2</sub> relative to the total number of determined particles increased, indicating that the summertime particles are more aged. Higher relative aerosol acidity (R<sub>ra</sub>) and lower in-situ pH (pH<sub>is</sub>) in summer suggest that particles are more acidic during this season. Correlation analysis and temporal variation characteristics suggest that from 9: 00 to 15: 00 in summer, C<sub>2</sub> particles mostly originate from the photochemical decomposition of larger dicarboxylic aids, driven by O<sub>3</sub> concentration. Conversely, from 16: 00 to 20: 00, C<sub>2</sub> particles are predominantly formed through aqueous-phase oxidation, influenced by higher relative humidity (RH), aerosol liquid water content (ALWC), and acidity. Additionally, heavy metal particles were the predominant type of C<sub>2</sub> particles, and C<sub>2</sub> particles exhibited an opposite diurnal variation to Fe in summer, suggesting that the photolysis of iron oxalate complexes is an important sink of C<sub>2</sub> particles during this period. In winter, biomass burning (BB) particles were the most abundant, and a robust correlation between levoglucosan and C<sub>2</sub> particles indicated a substantial influence of BB on C<sub>2</sub> particles. The aqueous generation of C<sub>2</sub> particles from α-dicarbonyls driven by acidity was most effective when RH varied from 40% to 60% in the wintertime state of particles. These findings highlight the hourly and seasonal variations in the sources and evolutionary processes of SOA. Such variations must be considered in developing control measures and simulating the climate effect of SOA.</div></div>","PeriodicalId":401,"journal":{"name":"Particuology","volume":"95 ","pages":"Pages 223-234"},"PeriodicalIF":4.1000,"publicationDate":"2024-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Mixing state and evolutionary mechanism of oxalic acid homologs in Liaocheng, East China: Insights from seasonal and hourly observations\",\"authors\":\"Jiangkai Ma , Jingjing Meng , Yanhui Wang , Xuan Liu , Xiaoting Zhang , Kaiyue Yang , Qiang Liu , Zhanfang Hou\",\"doi\":\"10.1016/j.partic.2024.09.011\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Oxalic acid (C<sub>2</sub>) is a significant tracer of secondary organic aerosols (SOA), yet its precursors, evolutionary processes, and formation mechanisms are not fully understood. This knowledge gap leads to uncertainties in evaluating the climate effect and global budget of SOA. Here we compared the size distribution, mixing fraction, and evolutionary mechanism of C<sub>2</sub>-containing particles between summer and winter. In summer, the number of C<sub>2</sub> particles and their homologs decreased compared to winter. However, the proportion of C<sub>2</sub> relative to the total number of determined particles increased, indicating that the summertime particles are more aged. Higher relative aerosol acidity (R<sub>ra</sub>) and lower in-situ pH (pH<sub>is</sub>) in summer suggest that particles are more acidic during this season. Correlation analysis and temporal variation characteristics suggest that from 9: 00 to 15: 00 in summer, C<sub>2</sub> particles mostly originate from the photochemical decomposition of larger dicarboxylic aids, driven by O<sub>3</sub> concentration. Conversely, from 16: 00 to 20: 00, C<sub>2</sub> particles are predominantly formed through aqueous-phase oxidation, influenced by higher relative humidity (RH), aerosol liquid water content (ALWC), and acidity. Additionally, heavy metal particles were the predominant type of C<sub>2</sub> particles, and C<sub>2</sub> particles exhibited an opposite diurnal variation to Fe in summer, suggesting that the photolysis of iron oxalate complexes is an important sink of C<sub>2</sub> particles during this period. In winter, biomass burning (BB) particles were the most abundant, and a robust correlation between levoglucosan and C<sub>2</sub> particles indicated a substantial influence of BB on C<sub>2</sub> particles. The aqueous generation of C<sub>2</sub> particles from α-dicarbonyls driven by acidity was most effective when RH varied from 40% to 60% in the wintertime state of particles. These findings highlight the hourly and seasonal variations in the sources and evolutionary processes of SOA. Such variations must be considered in developing control measures and simulating the climate effect of SOA.</div></div>\",\"PeriodicalId\":401,\"journal\":{\"name\":\"Particuology\",\"volume\":\"95 \",\"pages\":\"Pages 223-234\"},\"PeriodicalIF\":4.1000,\"publicationDate\":\"2024-09-25\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Particuology\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1674200124001858\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Particuology","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1674200124001858","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
Mixing state and evolutionary mechanism of oxalic acid homologs in Liaocheng, East China: Insights from seasonal and hourly observations
Oxalic acid (C2) is a significant tracer of secondary organic aerosols (SOA), yet its precursors, evolutionary processes, and formation mechanisms are not fully understood. This knowledge gap leads to uncertainties in evaluating the climate effect and global budget of SOA. Here we compared the size distribution, mixing fraction, and evolutionary mechanism of C2-containing particles between summer and winter. In summer, the number of C2 particles and their homologs decreased compared to winter. However, the proportion of C2 relative to the total number of determined particles increased, indicating that the summertime particles are more aged. Higher relative aerosol acidity (Rra) and lower in-situ pH (pHis) in summer suggest that particles are more acidic during this season. Correlation analysis and temporal variation characteristics suggest that from 9: 00 to 15: 00 in summer, C2 particles mostly originate from the photochemical decomposition of larger dicarboxylic aids, driven by O3 concentration. Conversely, from 16: 00 to 20: 00, C2 particles are predominantly formed through aqueous-phase oxidation, influenced by higher relative humidity (RH), aerosol liquid water content (ALWC), and acidity. Additionally, heavy metal particles were the predominant type of C2 particles, and C2 particles exhibited an opposite diurnal variation to Fe in summer, suggesting that the photolysis of iron oxalate complexes is an important sink of C2 particles during this period. In winter, biomass burning (BB) particles were the most abundant, and a robust correlation between levoglucosan and C2 particles indicated a substantial influence of BB on C2 particles. The aqueous generation of C2 particles from α-dicarbonyls driven by acidity was most effective when RH varied from 40% to 60% in the wintertime state of particles. These findings highlight the hourly and seasonal variations in the sources and evolutionary processes of SOA. Such variations must be considered in developing control measures and simulating the climate effect of SOA.
期刊介绍：
The word ‘particuology’ was coined to parallel the discipline for the science and technology of particles.
Particuology is an interdisciplinary journal that publishes frontier research articles and critical reviews on the discovery, formulation and engineering of particulate materials, processes and systems. It especially welcomes contributions utilising advanced theoretical, modelling and measurement methods to enable the discovery and creation of new particulate materials, and the manufacturing of functional particulate-based products, such as sensors.
Papers are handled by Thematic Editors who oversee contributions from specific subject fields. These fields are classified into: Particle Synthesis and Modification; Particle Characterization and Measurement; Granular Systems and Bulk Solids Technology; Fluidization and Particle-Fluid Systems; Aerosols; and Applications of Particle Technology.
Key topics concerning the creation and processing of particulates include:
-Modelling and simulation of particle formation, collective behaviour of particles and systems for particle production over a broad spectrum of length scales
-Mining of experimental data for particle synthesis and surface properties to facilitate the creation of new materials and processes
-Particle design and preparation including controlled response and sensing functionalities in formation, delivery systems and biological systems, etc.
-Experimental and computational methods for visualization and analysis of particulate system.
These topics are broadly relevant to the production of materials, pharmaceuticals and food, and to the conversion of energy resources to fuels and protection of the environment.
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