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Comparing respiratory aerosol emissions between children and adults during sustained phonation 比较儿童和成人在持续发声时的呼吸道气溶胶排放
4区 环境科学与生态学 Q2 ENGINEERING, CHEMICAL Pub Date : 2023-10-18 DOI: 10.1080/02786826.2023.2261715
Mahender Singh Rawat, Mehtap Agirsoy, Dinushani Senarathna, Byron D. Erath, Tanvir Ahmed, Sumona Mondal, Andrea R. Ferro
AbstractRespiratory aerosols arise due to bronchial fluid film bursting within the pulmonary tract, the vibration of the vocal folds during phonation, and articulation of the tongue/lips/teeth. We expect respiratory aerosol emission rates to be lower in children than adults due to the smaller size of their laryngeal structure, reduced sub-glottal pressure created during speech, and reduced number of alveoli. However, few studies have evaluated respiratory aerosols for children. We recruited 50 participants from three age categories: children aged 6−11 years, children aged 12−18 years, and adults ( >18 years). We investigated particle emissions for three different 5 s sustained vocalizations of /a/ or /pa/ at 262 Hz, as well as for running speech and breathing. The particle generation rate ranged from 0 to 488 particles/s. Children aged 6−11 years produced fewer particles (mean 12 ± SD 9 particles/s) than children aged 12−18 years (23 ± 19 particles/s) and adults (70 ± 73 particles/s). Taking a deep breath before vocalizing /a/ resulted in higher aerosol emission rates than the baseline case. The particle number size distributions for all vocalizations and age groups consistently showed two modes at ≈0.6 μm and ≈2 μm. Children had a slightly smaller primary mode location and larger secondary mode location than adults. Superemitters (statistical outliers) were found in all groups. Experiments repeated over time revealed large intrapersonal variability indicating additional variables (e.g., environmental, physiological, behavioral) may significantly influence emission rates. The lower respiratory aerosol emission rates for children indicate a need to consider population demographics when predicting airborne disease transmission risks.KEYWORDS: airborne particlesrespiratory emissionCOVID-19aerosolsbioaerosolstransmissionsuperemitterDisclaimerAs a service to authors and researchers we are providing this version of an accepted manuscript (AM). Copyediting, typesetting, and review of the resulting proofs will be undertaken on this manuscript before final publication of the Version of Record (VoR). During production and pre-press, errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal relate to these versions also. Additional informationFundingThis work was supported by the National Science Foundation [CBET:2029548] and the Clarkson University COVID-19 Special Solicitation.
摘要呼吸道气溶胶的产生是由于支气管液膜在肺部破裂、发声时声带的振动、舌/唇/齿的咬合等。我们预计儿童的呼吸道气溶胶排放率比成人低,因为他们的喉部结构较小,说话时产生的声门下压力减少,肺泡数量减少。然而,很少有研究对儿童呼吸道气溶胶进行评估。我们从三个年龄段招募了50名参与者:6 - 11岁的儿童、12 - 18岁的儿童和18岁以上的成年人。我们研究了在262hz下/a/或/pa/三种不同的持续5秒的发声,以及奔跑语音和呼吸时的颗粒排放。颗粒生成速率为0 ~ 488粒/s。6 ~ 11岁儿童产生的颗粒(平均12±SD 9颗粒/s)少于12 ~ 18岁儿童(23±19颗粒/s)和成人(70±73颗粒/s)。在发出/a/的声音之前深呼吸会导致比基线情况下更高的气溶胶排放率。在≈0.6 μm和≈2 μm处,各发声组和年龄组的粒径分布一致呈现出两种模式。与成人相比,儿童的主要模式位置略小,次要模式位置略大。在所有组中都发现了超级排放者(统计异常值)。随着时间的推移,反复进行的实验揭示了巨大的个人变异,表明其他变量(如环境、生理、行为)可能显著影响排放率。儿童呼吸道气溶胶排放率较低表明,在预测空气传播疾病的风险时,需要考虑人口统计学因素。关键词:空气颗粒呼吸排放covid -19气溶胶生物气溶胶传输超级发射器免责声明作为对作者和研究人员的服务,我们提供此版本的接受稿件(AM)。在最终出版版本记录(VoR)之前,将对该手稿进行编辑、排版和审查。在制作和印前,可能会发现可能影响内容的错误,所有适用于期刊的法律免责声明也与这些版本有关。本研究得到了美国国家科学基金[CBET:2029548]和克拉克森大学COVID-19特别征集的支持。
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引用次数: 0
Estimating Viscosity of Individual Substrate-Deposited Particles from Measurements of Their Height-to-Width Ratios 从测量其高宽比估计单个基底沉积颗粒的粘度
4区 环境科学与生态学 Q2 ENGINEERING, CHEMICAL Pub Date : 2023-10-16 DOI: 10.1080/02786826.2023.2270503
Felipe A. Rivera-Adorno, Jay M. Tomlin, Matthew Fraund, Erick Morgan, Michael Laskin, Ryan Moffet, Alexander Laskin
AbstractAirborne particles alter the radiative forcing of climate and have further consequences on air visibility, atmospheric chemistry, and human health. Recent studies reported the existence of highly viscous semi-solid and even solid amorphous organic aerosol (OA) particles. Particle viscosity has an impact on the heterogeneous chemistry, gas-particle partitioning, and ice nucleation properties. Consequently, variations in particle viscosity must be considered when predicting the atmospheric impact of OA. Here we use scanning electron microscopy (SEM) and scanning transmission X-ray microscopy (STXM) to estimate the viscosity of individual particles deposited on substrates based on their characteristic height-to-width ratios, which are affected by changes in morphology upon deposition. The height-to-width ratios obtained from SEM and STXM exhibit a strong correlation, demonstrating that both imaging approaches can be applied separately for viscosity assessment of the substrate-deposited particles. While these metrics are largely qualitative, this method enables rapid assessment of particle viscosity ranges, distinguishing between semi-solid (>1010 Pa·s), viscous (104-108 Pa·s), and liquid (10°-101 Pa·s) particles within ensembles of ambient particles collected for microscopy studies.DisclaimerAs a service to authors and researchers we are providing this version of an accepted manuscript (AM). Copyediting, typesetting, and review of the resulting proofs will be undertaken on this manuscript before final publication of the Version of Record (VoR). During production and pre-press, errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal relate to these versions also. AcknowledgementsThis work was supported by the U. S. Department of Energy’s (DOE) Atmospheric System Research program, Office of Biological and Environmental Research (OBER), award DE-SC0021977. The SEM imaging for this project was performed at the Life Science Microscope Facility at Purdue University. The STXM imaging was performed at beamline 5.3.2.2 of the Advanced Light Source at Lawrence Berkeley National Laboratory. We thank Mr. Mark Carlsen, instrumentation specialist from Purdue’s Jonathan Amy Facility for Chemical Instrumentation, for assembling the drying system used for particle generation and collection.Author contributionsF.R. and A.L. devised the project. F.R., J.T., M.F., R.M. conducted STXM measurements. F. R. and E.M. conducted laboratory experiments, collected samples of particle standards, performed SEM measurements, analyzed and integrated all datasets. M.L. provided geometry derivations. F.R. and A.L. wrote the manuscript with contributions from all coauthors. The authors report there are no competing interests to declare.
摘要空气粒子改变了气候的辐射强迫,并对空气能见度、大气化学和人类健康产生了进一步的影响。近年来的研究报道了高粘性半固态甚至固态非晶有机气溶胶(OA)颗粒的存在。颗粒粘度对非均相化学、气粒分配和冰核性质有影响。因此,在预测OA对大气的影响时,必须考虑颗粒粘度的变化。在这里,我们使用扫描电子显微镜(SEM)和扫描透射x射线显微镜(STXM)来估计沉积在衬底上的单个颗粒的粘度,基于它们的特征高宽比,这受沉积时形貌变化的影响。从SEM和STXM获得的高宽比显示出很强的相关性,表明这两种成像方法可以单独应用于基材沉积颗粒的粘度评估。虽然这些指标在很大程度上是定性的,但该方法可以快速评估颗粒粘度范围,区分为显微镜研究收集的环境颗粒集合中的半固体(>1010 Pa·s),粘性(104-108 Pa·s)和液体(10°-101 Pa·s)颗粒。免责声明作为对作者和研究人员的服务,我们提供了这个版本的已接受的手稿(AM)。在最终出版版本记录(VoR)之前,将对该手稿进行编辑、排版和审查。在制作和印前,可能会发现可能影响内容的错误,所有适用于期刊的法律免责声明也与这些版本有关。本工作得到了美国能源部(DOE)大气系统研究项目、生物与环境研究办公室(OBER)的资助,项目编号为DE-SC0021977。该项目的扫描电镜成像是在普渡大学的生命科学显微镜设施进行的。STXM成像在劳伦斯伯克利国家实验室先进光源的光束线5.3.2.2处进行。我们感谢来自普渡大学乔纳森·艾米化学仪器设备的仪器专家马克·卡尔森先生,他组装了用于颗粒产生和收集的干燥系统。作者contributionsF.R。A.L.设计了这个项目。f.r., j.t., m.f., R.M.进行STXM测量。f.r.和E.M.进行了实验室实验,收集了颗粒标准样品,进行了扫描电镜测量,分析并整合了所有数据集。M.L.提供几何推导。F.R.和A.L.在所有共同作者的贡献下撰写了这份手稿。作者报告说,没有相互竞争的利益需要申报。
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引用次数: 0
Probing the pH dependence of brown carbon formation: Insights from laboratory studies on aerosol particles and bulk phase solutions 探索棕碳形成的pH依赖性:来自气溶胶颗粒和本体相溶液的实验室研究的见解
4区 环境科学与生态学 Q2 ENGINEERING, CHEMICAL Pub Date : 2023-10-10 DOI: 10.1080/02786826.2023.2267649
Kevin T. Jansen, Margaret A. Tolbert
AbstractLight-absorbing organic aerosol (brown carbon, BrC) can have a significant impact on the radiative balance of the Earth’s atmosphere. However there are still substantial uncertainties regarding the formation, composition, and radiative properties of BrC. In this study, we conducted laboratory experiments to investigate the pH dependence of BrC formation in both aerosol particles and bulk phase solutions. Using glyoxal, ammonia, and ammonium salts, we generated precursor solutions under varying bulk pH conditions ranging from 0.69 to 8.43. Drying the solutions either in the bulk or aerosol phase resulted in BrC formation. The resulting organic material was analyzed to determine its chemical composition and optical properties. Under the set of conditions investigated here, neutral to basic conditions of relevance to cloud water favored BrC formation for both aerosols and bulk solutions. In contrast, BrC products were formed under acidic conditions only in the aerosol phase. Due to rapid equilibration with the gas phase and evaporative losses of water, the aerosols probed here likely had extremely low pH values, well below the bulk pH of 0.69. By achieving such acidic conditions in the aerosol phase, new acid-catalyzed pathways are possible to form BrC. These findings indicate brown carbon formation is favored at both high and very low pH, and further point to the importance of using aerosol samples in studies of pH dependent chemistry of relevance to the atmosphere.DisclaimerAs a service to authors and researchers we are providing this version of an accepted manuscript (AM). Copyediting, typesetting, and review of the resulting proofs will be undertaken on this manuscript before final publication of the Version of Record (VoR). During production and pre-press, errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal relate to these versions also.
摘要吸光有机气溶胶(brown carbon, BrC)对地球大气的辐射平衡具有重要影响。然而,关于BrC的形成、组成和辐射特性仍然存在大量的不确定性。在这项研究中,我们进行了实验室实验,研究了气溶胶颗粒和体相溶液中BrC形成的pH依赖性。使用乙二醛,氨和铵盐,我们在不同的体积pH值条件下生成前体溶液,范围从0.69到8.43。在散装或气溶胶阶段干燥的溶液导致BrC的形成。对所得的有机材料进行了分析,以确定其化学成分和光学性质。在这里研究的一系列条件下,与云水相关的中性和基本条件有利于气溶胶和散装溶液的BrC形成。相比之下,BrC产物在酸性条件下仅在气溶胶相形成。由于与气相的快速平衡和水的蒸发损失,这里探测的气溶胶可能具有极低的pH值,远低于0.69的体积pH值。通过在气溶胶相中达到这样的酸性条件,新的酸催化途径可能形成BrC。这些发现表明,棕色碳的形成在高和极低的pH值下都是有利的,并进一步指出了在研究与大气相关的pH依赖性化学中使用气溶胶样品的重要性。免责声明作为对作者和研究人员的服务,我们提供了这个版本的已接受的手稿(AM)。在最终出版版本记录(VoR)之前,将对该手稿进行编辑、排版和审查。在制作和印前,可能会发现可能影响内容的错误,所有适用于期刊的法律免责声明也与这些版本有关。
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引用次数: 0
The Filtration Efficiency of Surgical Masks for Expiratory Aerosol and Droplets Generated by Vocal Exercises 外科口罩对发声练习产生的呼气气雾和飞沫的过滤效率
4区 环境科学与生态学 Q2 ENGINEERING, CHEMICAL Pub Date : 2023-10-10 DOI: 10.1080/02786826.2023.2267689
Alicja Szczepanska, Joshua Harrison, Brian Saccente-Kennedy, Justice Archer, Natalie A. Watson, Christopher M. Orton, William J. Browne, Ruth Epstein, James D. Calder, Pallav L. Shah, Declan Costello, Bryan R. Bzdek, Jonathan P. Reid
AbstractTransmission of an airborne disease can occur when an individual exhales respiratory particles that contain infectious pathogens. Surgical face masks are often used to reduce the amount of respiratory aerosol emitted into the environment by an individual while also lowering the concentration of particles the individual inhales. Respiratory aerosol generation is activity-dependent with high person-to-person variability. Moreover, mask fit differs among people. Here, we measure the efficacy of surgical masks (EN14683 Type IIR) in reducing both aerosol (0.3 – 20 μm diameter) and droplet (20 – 1000 μm diameter) emission during breathing, speaking and five speech and language therapy tasks performed by a human cohort. When participants wore a surgical face mask, measured particle number concentrations at the front of the mask were always lower than that for breathing without mitigation in place. For breathing and speaking, the through-mask filtration efficiencies were 80% and 87%, respectively, while for voice therapy tasks the through-mask filtration efficiencies ranged from 89% (“Hey!”) to 95% (/a::/). Size-dependent through-mask filtration efficiencies were high (80 – 95%) for particles 0.5 – 2 μm diameter, with masks filtering a greater fraction of larger particle sizes. For particle sizes >4 µm diameter, filtration efficiencies of surgical face masks for all tested respiratory tasks were ∼100%. Surgical face masks significantly reduced the number of particles emitted from all respiratory activities. These results have implications for developing effective mitigations for diseases transmission through inhalation.DisclaimerAs a service to authors and researchers we are providing this version of an accepted manuscript (AM). Copyediting, typesetting, and review of the resulting proofs will be undertaken on this manuscript before final publication of the Version of Record (VoR). During production and pre-press, errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal relate to these versions also. ACKNOWLEDGEMENTSThe authors acknowledge funding from the Engineering and Physical Sciences Research Council (EP/V050516/1). B.R.B. acknowledges the Natural Environment Research Council (NE/P018459/1). B.R.B. and A.S. acknowledge funding from the European Research Council (Project 948498, AeroSurf). J.H. acknowledges funding from the EPSRC Centre for Doctoral Training in Aerosol Science (EP/S023593/1). Fortius Surgical Centre, Marylebone, London, is acknowledged for the generous provision of space to conduct the measurements. We thank all our volunteer participants for their contribution to this study.Data AvailabilityData underlying the figures are publicly available in the BioStudies database (https://www.ebi.ac.uk/biostudies/) under accession ID S-BSST1187.The analysed data are provided in Supplemental Information available online.
当一个人呼出含有传染性病原体的呼吸道颗粒时,就会发生空气传播疾病。外科口罩通常用于减少个人向环境中排放的呼吸道气溶胶的数量,同时也降低个人吸入的颗粒浓度。呼吸道气溶胶的产生依赖于活动,具有高度的人与人之间的可变性。此外,口罩适合度因人而异。在这里,我们测量了外科口罩(EN14683型IIR)在呼吸、说话和五项言语和语言治疗任务中减少气溶胶(0.3 - 20 μm直径)和液滴(20 - 1000 μm直径)排放的功效。当参与者戴上外科口罩时,口罩前部测量到的颗粒数浓度总是低于没有缓解措施的呼吸。对于呼吸和说话,通过面罩过滤效率分别为80%和87%,而对于语音治疗任务,通过面罩过滤效率从89%(“嘿!”)到95% (/a::/)不等。对于直径为0.5 ~ 2 μm的颗粒,粒径相关的掩膜过滤效率高达80 ~ 95%,对于较大粒径的颗粒,掩膜过滤的比例更高。对于粒径>4µm的颗粒,外科口罩对所有测试呼吸任务的过滤效率为~ 100%。外科口罩显著减少了所有呼吸活动释放的颗粒数量。这些结果对制定通过吸入传播疾病的有效缓解措施具有启示意义。免责声明作为对作者和研究人员的服务,我们提供了这个版本的已接受的手稿(AM)。在最终出版版本记录(VoR)之前,将对该手稿进行编辑、排版和审查。在制作和印前,可能会发现可能影响内容的错误,所有适用于期刊的法律免责声明也与这些版本有关。作者感谢工程与物理科学研究委员会(EP/V050516/1)的资助。B.R.B.感谢自然环境研究委员会(NE/P018459/1)。B.R.B.和A.S.承认来自欧洲研究委员会的资助(项目948498,AeroSurf)。J.H.承认EPSRC气溶胶科学博士培训中心(EP/S023593/1)的资助。Fortius外科中心,Marylebone,伦敦,是公认的慷慨提供空间进行测量。我们感谢所有志愿者对这项研究的贡献。数据可获得性数据基础数据可在BioStudies数据库(https://www.ebi.ac.uk/biostudies/)公开获取,登录ID为S-BSST1187。分析的数据在网上提供的补充信息中提供。
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引用次数: 0
Impact of Test Methodology on the Efficacy of Triethylene Glycol (Grignard Pure) against Bacteriophage MS2 试验方法对三甘醇(格氏纯品)抗噬菌体MS2效果的影响
4区 环境科学与生态学 Q2 ENGINEERING, CHEMICAL Pub Date : 2023-10-09 DOI: 10.1080/02786826.2023.2262004
Katherine M. Ratliff, Lukas Oudejans, John Archer, Worth Calfee, Jerome U. Gilberry, David Adam Hook, William E. Schoppman, Robert W. Yaga, Lance Brooks, Shawn Ryan
AbstractThe COVID-19 pandemic has raised interest in using chemical air treatments as part of a strategy to reduce the risk of disease transmission, but more information is needed to characterize their efficacy at scales translatable to applied settings and to develop standardized test methods for characterizing the performance of these products. Grignard Pure, a triethylene glycol (TEG) active ingredient air treatment, was evaluated using two different test protocols in a large bioaerosol test chamber and observed to inactivate bacteriophage MS2 in air (up to 99.9% at 90 minutes) and on surfaces (up to 99% at 90 minutes) at a concentration of approximately 1.2 – 1.5 mg/m3. Introducing bioaerosol into a TEG-charged chamber led to overall greater reductions compared to when TEG was introduced into a bioaerosol-charged chamber, although the differences in efficacy against airborne MS2 were only significant in the first 15 minutes. Time-matched control conditions (no TEG present) and replicate tests for each condition were essential for characterizing treatment efficacy. These findings suggest that chemical air treatments could be effective in reducing the air and surface concentrations of infectious pathogens in occupied spaces, although standard methods are needed for evaluating their efficacy and comparing results across studies. The potential health impacts of chronic exposure to chemicals should also be considered, but those were not evaluated here.DisclaimerAs a service to authors and researchers we are providing this version of an accepted manuscript (AM). Copyediting, typesetting, and review of the resulting proofs will be undertaken on this manuscript before final publication of the Version of Record (VoR). During production and pre-press, errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal relate to these versions also. AcknowledgementsThe authors gratefully acknowledge members of the EPA Project Team, the members of Jacobs Technology, Inc. (JTI) supporting the EPA Homeland Security and Materials Management Microbiology lab and the JTI Aerosol Science Team, Adam Burdsall and Marc Carpenter for internal technical reviews of this manuscript, and Ramona Sherman and for quality assurance support.DisclaimerThe EPA, through its Office of Research and Development, directed the research described herein conducted through contract 68HERC20D0018 with Jacobs Technology, Inc. It has been subjected to the Agency's review and has been approved for publication. Mention of trade names, products or services does not convey official EPA approval, endorsement, or recommendation.Declaration of InterestsThe authors report there are no competing interests to declare.Data AvailabilityThe data that support the findings of this study are openly available at https://doi.org/10.23719/1528421.
摘要2019冠状病毒病大流行引起了人们对使用化学空气处理作为降低疾病传播风险战略的一部分的兴趣,但需要更多的信息来表征其可转化为应用环境的规模的功效,并开发标准化测试方法来表征这些产品的性能。Grignard Pure是一种三乙二醇(TEG)活性成分空气处理方法,在大型生物气溶胶测试室中使用两种不同的测试方案进行了评估,并观察到在空气(90分钟达99.9%)和表面(90分钟达99%)中,浓度约为1.2 - 1.5 mg/m3时,噬菌体MS2的灭活效果。与将TEG引入充满生物气溶胶的房间相比,将生物气溶胶引入充满TEG的房间导致总体上更大的减少,尽管对空气中MS2的功效差异仅在前15分钟内显着。时间匹配的对照条件(不存在TEG)和每个条件的重复试验是表征治疗效果的必要条件。这些发现表明,化学空气处理可以有效地降低被占用空间中传染性病原体的空气和表面浓度,尽管需要标准方法来评估其功效并比较研究结果。长期接触化学品对健康的潜在影响也应加以考虑,但这里没有对这些影响进行评估。免责声明作为对作者和研究人员的服务,我们提供了这个版本的已接受的手稿(AM)。在最终出版版本记录(VoR)之前,将对该手稿进行编辑、排版和审查。在制作和印前,可能会发现可能影响内容的错误,所有适用于期刊的法律免责声明也与这些版本有关。作者感谢EPA项目团队成员,雅各布斯技术公司(JTI)支持EPA国土安全和材料管理微生物实验室和JTI气溶胶科学团队的成员,Adam Burdsall和Marc Carpenter对本文的内部技术审查,以及Ramona Sherman和质量保证支持。美国环境保护署通过其研究与发展办公室,根据合同68HERC20D0018与Jacobs Technology, Inc.进行了本文所述的研究。该报告已经过原子能机构的审查,并已获准出版。提及商品名称、产品或服务并不表示官方的EPA批准、认可或推荐。利益声明作者报告没有竞争利益需要申报。数据可用性支持本研究结果的数据可在https://doi.org/10.23719/1528421上公开获取。
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引用次数: 0
The volatility of pollen extracts and their main constituents in aerosolized form via the integrated volume method (IVM) and the volatility basis set (VBS) 利用积分体积法(IVM)和挥发性基集(VBS)研究花粉提取物及其主要成分的挥发性。
4区 环境科学与生态学 Q2 ENGINEERING, CHEMICAL Pub Date : 2023-10-06 DOI: 10.1080/02786826.2023.2265954
Kevin Axelrod, Chiranjivi Bhattarai, Palina Bahdanovich, Vera Samburova, Andrey Y. Khlystov
The volatility of organic aerosol in the atmosphere is an important quality that determines the aerosol/gas partitioning of compounds in the atmosphere and thus influences their ability to participate in gas-phase reactions in the atmosphere. In this research, the volatility of biological aerosols, specifically water-soluble pollen extracts and their chemical constituents, are studied for important thermodynamic properties such as saturation vapor concentration and latent heat of vaporization. The integrated volume method (IVM) was applied to characterize these properties for various free amino acids and saccharides in pollen, and the volatility basis set (VBS) approach was utilized to obtain a distribution of the mass fraction of pollen extracts with respect to saturation vapor concentration. Our results indicate that among seven compounds tested with the IVM, proline, γ-aminobutyric acid, and fructose had semivolatile saturation vapor concentrations of 17.5 ± 2.2, 14.7 ± 0.8, and 4.4 ± 0.5 μg m−3, respectively. Additionally, our VBS measurements indicate that aspen pollen extract contains a greater semivolatile mass fraction (up to 8.5% of total water-soluble mass) than lodgepole pine pollen (up to 2.2%), indicating that different pollen species may contribute to the total atmospheric semivolatile organic compound (SVOC) and low volatile organic compound (LVOC) budget differently. Depending on estimates of several factors, fluxes and concentrations of SVOCs and LVOCs from pollen could be comparable to other sources such as biomass burning and ambient urban emissions, though further research is needed to better constrain the contribution of pollen and other bioaerosols to organic compounds in the atmosphere.
大气中有机气溶胶的挥发性是决定大气中化合物的气溶胶/气体分配从而影响其参与大气中气相反应的能力的重要品质。在本研究中,生物气溶胶,特别是水溶性花粉提取物及其化学成分的挥发性,研究了重要的热力学性质,如饱和蒸汽浓度和汽化潜热。利用积分体积法(IVM)表征花粉中各种游离氨基酸和糖类的这些性质,利用挥发性基集(VBS)方法获得花粉提取物的质量分数相对于饱和蒸汽浓度的分布。结果表明,在IVM测试的7种化合物中,脯氨酸、γ-氨基丁酸和果糖的半挥发性饱和蒸汽浓度分别为17.5±2.2、14.7±0.8和4.4±0.5 μ m−3。此外,我们的VBS测量结果表明,白杨花粉提取物含有更高的半挥发性质量分数(占总水溶性质量的8.5%),而白杨花粉提取物含有更高的半挥发性质量分数(占总水溶性质量的2.2%),这表明不同的花粉种类可能对大气总半挥发性有机化合物(SVOC)和低挥发性有机化合物(LVOC)预算有不同的贡献。根据对若干因素的估计,来自花粉的SVOCs和LVOCs的通量和浓度可与其他来源(如生物质燃烧和城市环境排放)相媲美,尽管需要进一步研究以更好地限制花粉和其他生物气溶胶对大气中有机化合物的贡献。
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引用次数: 0
Optimization of sampling conditions to minimize sampling errors of both PM 2.5 mass and its semi-volatile inorganic ion concentrations 优化采样条件,使pm2.5质量及其半挥发性无机离子浓度的采样误差最小化
4区 环境科学与生态学 Q2 ENGINEERING, CHEMICAL Pub Date : 2023-10-06 DOI: 10.1080/02786826.2023.2265454
Thi-Cuc Le, Pallavi Gajanan Barhate, Kai-Jing Zhen, Manisha Mishra, David. Y. H. Pui, Chuen-Jinn Tsai
ABSTRACTThe accurate measurement of PM2.5 and its inorganic matters (IMs) is crucial for compliance monitoring and understanding particle formation. However, semi-volatile IMs (SVIMs) like NH4+, NO3− and Cl− tend to evaporate from particles, causing sampling artifacts. The evaporation loss occurs due to many factors making the quantitative prediction difficult. This study aimed to investigate the evaporation loss of SVIMs in PM2.5 under different sampling conditions. In the field tests, when a normal single Teflon filter sampler (STF), which is like a Federal Reference Method (FRM) sampler, was used to sample PM2.5 at ambient conditions, a significant SVIM evaporation loss was observed, resulting in negative biases for total IMs (-25.68 ± 3.25%) and PM2.5 concentrations (-9.87 ± 4.27%). But if PM2.5 was sampled by a chilled Teflon filter sampler (CTF) at 4 0C following aerosol dehumidification so that relative humidity (RH) was controlled to within the 10-20% range (RHd), evaporation loss was minimized with a bias of < ±10% for both total IMs and PM2.5 based on the reference data. When RHd is below 10%, both IMs and PM2.5 are under-measured, but only PM2.5 is over-measured when RHd is >20%. A model considering predictable saturation ratios for NH4+, NO3− and Cl− under various pressure drop, temperature and RH conditions was developed to predict accurately the actual concentrations of PM2.5 and its SVIMs for the STF. Additionally, the ISORROPIA-II model predicted SVIMs effectively for the CTF. In summary, using the CTF at optimized sampling conditions can achieve accurate measurement of both SVIMs and PM2.5 concentrations simultaneously.DisclaimerAs a service to authors and researchers we are providing this version of an accepted manuscript (AM). Copyediting, typesetting, and review of the resulting proofs will be undertaken on this manuscript before final publication of the Version of Record (VoR). During production and pre-press, errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal relate to these versions also. AcknowledgementsThis work was supported by the Ministry of Science and Technology, Taiwan (contract MOST 111-2221-E-A49-057-MY3), the Ministry of Education, the Higher Education Sprout Project of National Yang Ming Chiao Tung University, and the Academic-Industry Research Hub of People and Earth (AIR HoPE).Disclosure statementThe authors report there are no competing interests to declare.
摘要PM2.5及其无机物(IMs)的准确测量对于合规监测和了解颗粒形成至关重要。然而,NH4+, NO3 -和Cl -等半挥发性IMs (SVIMs)倾向于从颗粒中蒸发,导致采样伪影。蒸发损失的发生受多种因素的影响,使定量预测变得困难。本研究旨在探讨不同采样条件下PM2.5中svm的蒸发损失。在现场试验中,当使用类似于联邦参考法(FRM)采样器的普通单Teflon过滤器采样器(STF)在环境条件下采样PM2.5时,观察到明显的SVIM蒸发损失,导致总IMs(-25.68±3.25%)和PM2.5浓度(-9.87±4.27%)呈负偏差。但是,如果在气溶胶除湿后,在4℃的温度下使用冷冻聚四氟乙烯过滤器采样器(CTF)采样PM2.5,使相对湿度(RH)控制在10-20%的范围内(RHd),则根据参考数据,总IMs和PM2.5的蒸发损失都最小,偏差<±10%。当RHd < 10%时,IMs和PM2.5均偏低,当RHd >20%时,只有PM2.5超标。建立了一个考虑不同压降、温度和相对湿度条件下NH4+、NO3−和Cl−可预测饱和比的模型,以准确预测STF的PM2.5实际浓度及其svm。此外,ISORROPIA-II模型有效地预测了CTF的svm。综上所述,在优化的采样条件下使用CTF可以同时准确测量svm和PM2.5浓度。免责声明作为对作者和研究人员的服务,我们提供了这个版本的已接受的手稿(AM)。在最终出版版本记录(VoR)之前,将对该手稿进行编辑、排版和审查。在制作和印前,可能会发现可能影响内容的错误,所有适用于期刊的法律免责声明也与这些版本有关。本工作得到台湾科学技术部(合同编号:MOST 111-2221-E-A49-057-MY3)、教育部、国立阳明交通大学高等教育育苗计划、人与地球产学研中心(AIR HoPE)的支持。作者报告无利益竞争需要申报。
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引用次数: 0
Multi-modal Chemical Characterization of Highly Viscous Submicrometer Organic Particles. 高粘性亚微米有机颗粒的多模态化学表征。
4区 环境科学与生态学 Q2 ENGINEERING, CHEMICAL Pub Date : 2023-10-05 DOI: 10.1080/02786826.2023.2266494
Ana C. Morales, Brianna N. Peterson, Steven A. Sharpe, Shelby M. Huston, Jay M. Tomlin, Felipe A. Rivera-Adorno, Ryan C. Moffet, Alla Zelenyuk, Alexander Laskin
AbstractDistinguishing highly viscous organic particles within complex mixtures of atmospheric aerosol and accurate descriptions of their composition, size distributions, and mixing states are challenges at the forefront of aerosol measurement science and technology. Here, we present results obtained from complementary single-particle measurement techniques employed for the in-depth characterization of highly viscous particles. We demonstrate advantages and synergy of this multi-modal particle characterization approach based on the analysis of individual viscous particles formed in the air-discharged waste produced by a common sewer pipe rehabilitation technology. Using oil immersion flow microscopy, we investigate particle size distributions and morphology of colloidal components present in field-collected aqueous waste condensates. We compare these results with corresponding measurements of viscous particles formed in drying droplets of the aerosolized discharged waste. The colloidal components and viscous particles were found to be approximately 10 µm and 0.5 µm, respectively. The aerosolized viscous particles exhibited a spherical morphology, while the colloidal particles appeared noticeably fractal, resembling fragments of a cured composite material. Chemical imaging of the viscous particles collected on substrates was performed using scanning electron microscopy and soft X-ray spectro-microscopy techniques. Through these methods, comprehensive description of these particles emerged, confirming their high solid-like viscosity, wide-ranging sizes, diverse carbon speciation with high degrees of oxygenation, and high organic volume fractions. The aerosolized viscous particles were further characterized using high-throughput single particle mass spectrometry. This technique provides real-time measurements of composition, size, and morphological metrics for large numbers of individual particles, enabling the identification of their distinct mass spectrometric signatures.DisclaimerAs a service to authors and researchers we are providing this version of an accepted manuscript (AM). Copyediting, typesetting, and review of the resulting proofs will be undertaken on this manuscript before final publication of the Version of Record (VoR). During production and pre-press, errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal relate to these versions also.
摘要在复杂的大气气溶胶混合物中识别高粘性有机颗粒并准确描述其组成、大小分布和混合状态是气溶胶测量科学和技术的前沿挑战。在这里,我们提出了从用于深入表征高粘性颗粒的互补单颗粒测量技术获得的结果。我们展示了这种多模态颗粒表征方法的优势和协同作用,该方法基于对一种常见污水管道修复技术产生的空气排放废物中形成的单个粘性颗粒的分析。利用油浸流动显微镜,我们研究了现场收集的废水凝析油中胶体组分的粒径分布和形态。我们将这些结果与相应的测量结果进行比较,这些测量结果是在雾化排放的废物的干燥液滴中形成的粘性颗粒。胶体成分和粘性颗粒分别约为10µm和0.5µm。雾化后的粘性颗粒呈球形形态,而胶体颗粒呈明显的分形,类似于固化复合材料的碎片。利用扫描电子显微镜和软x射线光谱显微镜技术对收集在衬底上的粘性颗粒进行化学成像。通过这些方法,对这些颗粒进行了全面的描述,证实了它们具有高固体样粘度、广泛的尺寸、多样的碳形态和高度的氧化性以及高有机体积分数。采用高通量单粒子质谱法进一步表征了雾化后的粘性颗粒。该技术可以实时测量大量单个颗粒的组成、大小和形态指标,从而识别它们不同的质谱特征。免责声明作为对作者和研究人员的服务,我们提供了这个版本的已接受的手稿(AM)。在最终出版版本记录(VoR)之前,将对该手稿进行编辑、排版和审查。在制作和印前,可能会发现可能影响内容的错误,所有适用于期刊的法律免责声明也与这些版本有关。
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引用次数: 0
Effects of volatility, viscosity, and non-ideality on particle–particle mixing timescales of secondary organic aerosols 挥发性、粘度和非理想性对二次有机气溶胶颗粒-颗粒混合时间尺度的影响
4区 环境科学与生态学 Q2 ENGINEERING, CHEMICAL Pub Date : 2023-09-26 DOI: 10.1080/02786826.2023.2256827
Meredith Schervish, Neil M Donahue, Manabu Shiraiwa
Different populations of aerosol are constantly mixed throughout the atmosphere. Large-scale models often assume no particle–particle mixing or fast mixing among aerosol populations, so that they stay externally mixed or instantaneously form internal mixtures. We apply the kinetic multilayer model of gas–particle interactions (KM-GAP) to simulate the evaporation of semi-volatile species from one particle population and partitioning into another population with various phase states and nonideal mixing conditions. We find that the particle–particle mixing timescale (τmix) is prolonged when the semi-volatile species transport to a population in which it is miscible, as more mass must be transported. Extremes of volatility prolong the τmix, as low-volatility species evaporate slowly, while high-volatility species condense slowly. When the bulk diffusivities of the two populations are greater than 10−15 cm2 s−1, semi-volatile species mix rapidly; otherwise, the τmix can be prolonged beyond 1 h. We apply KM-GAP to particle–particle mixing experiments of H-toluene SOA into D-toluene SOA and limonene SOA, showing that τmix is prolonged when toluene SOA is highly viscous, while initial partitioning of gas phase semi-volatile species from toluene SOA into limonene SOA is rapid because of the low viscosity of limonene SOA. Simulations of mixing toluene SOA and β-caryophyllene SOA indicate that the apparent discrepancy of limited mixing under conditions where both are predicted to have low viscosity are explained by limited miscibility of the semi-volatile components. Our study demonstrates that particle–particle mixing timescales are affected by a complex interplay among volatility, diffusion limitations, and non-ideal miscibility.
不同种类的气溶胶在大气中不断混合。大尺度模型通常假设气溶胶种群之间没有粒子-粒子混合或快速混合,因此它们保持外部混合或立即形成内部混合。我们应用气-粒子相互作用动力学多层模型(KM-GAP)模拟了在不同相态和非理想混合条件下,半挥发性物质从一个粒子群中蒸发到另一个粒子群中的过程。我们发现,当半挥发性物质迁移到可混溶的种群时,粒子-粒子混合时间标度τmix会延长,因为必须迁移更多的质量。波动率的极值延长了τ混合物,因为低波动率的物种蒸发缓慢,而高波动率的物种凝结缓慢。当两个种群的体积扩散系数大于10 ~ 15 cm2 s−1时,半挥发性物种混合迅速;我们将KM-GAP应用于h -甲苯SOA与d -甲苯SOA和柠檬烯SOA的粒子-粒子混合实验,结果表明,当甲苯SOA粘度高时,τ混合时间延长,而由于柠檬烯SOA粘度低,气相半挥发性物质从甲苯SOA到柠檬烯SOA的初始分解速度很快。混合甲苯SOA和β-石竹烯SOA的模拟表明,在预测两者具有低粘度的条件下,有限混合的明显差异可以用半挥发性组分的有限混相来解释。我们的研究表明,颗粒-颗粒混合时间尺度受到挥发性、扩散限制和非理想混相之间复杂的相互作用的影响。
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引用次数: 0
Detection of sub-5nm naturally charged carbonaceous materials from a sooting laminar premixed flame by a water condensation Particle Counter (WCPC) enhanced by a Di-Ethylene Glycol (DEG) saturator inlet 通过二乙二醇(DEG)饱和器入口增强的水冷凝颗粒计数器(WCPC)检测来自烟熏层流预混火焰的亚5nm天然带电碳质材料
IF 5.2 4区 环境科学与生态学 Q2 ENGINEERING, CHEMICAL Pub Date : 2023-09-07 DOI: 10.1080/02786826.2023.2247458
Farnaz Khosravi, Gregory S. Lewis, Michel Attoui, Arantza Eiguren-Fernandez, Francesco Carbone
Abstract Combustion is one of the major contributors to air pollution and Condensation Particle Counters (CPCs) provide effective monitoring of atmospheric aerosols since they can detect both charged and neutral materials in low number concentrations. The detection efficiency of any CPC for materials smaller than 5 nm requires ad-hoc calibrations because it is affected by the analyte’s size, shape, charge state, composition, and wettability by the condensing fluid. This study characterizes a Water-based CPC (WCPC) prototype for the detection of the naturally charged carbonaceous products of an incipiently sooting laminar premixed flame. The WCPC can activate condensation growth and (50% efficient) detection of hydrophobic flame-formed carbonaceous materials naturally charged in positive and negative polarities with mobility diameters as small as 4.3 nm and 4.8 nm, respectively. The addition of a simple Di-Ethylene Glycol (DEG) saturator inlet enhances the 50% detection cutoff to mobility diameters as small as 1.8 nm or 1.6 nm for materials charged in positive or negative polarity, respectively. The coupling of the DEG saturator inlet to the WCPC creates a new DEG-WCPC instrument able to detect efficiently both hydrophobic and hydrophilic sub-5nm aerosols with a marginal increase in manufacturing cost (<10%), dimensions, and weight (<0.25 kg). Copyright © 2023 American Association for Aerosol Research Graphical Abstract
摘要燃烧是造成空气污染的主要原因之一,冷凝粒子计数器(CPC)可以检测低浓度的带电和中性物质,因此可以有效监测大气气溶胶。任何CPC对小于5的材料的检测效率 nm需要特别校准,因为它受到分析物的大小、形状、电荷状态、成分和冷凝流体的润湿性的影响。这项研究表征了一个水基CPC(WCPC)原型,用于检测初始吹灰层流预混火焰的天然带电碳质产物。WCPC可以激活缩合生长,并(50%有效)检测疏水性火焰形成的碳质材料,这些碳质材料以正负极性自然带电,迁移率直径小至4.3 nm和4.8 nm。添加一个简单的二乙二醇(DEG)饱和器入口,可将50%的检测截止值提高到小至1.8的迁移率直径 nm或1.6 对于以正极性或负极性充电的材料分别为nm。DEG饱和器入口与WCPC的耦合创造了一种新的DEG-WCPC仪器,能够有效检测疏水性和亲水性亚5nm气溶胶,制造成本(<10%)、尺寸和重量(<0.25 kg)。版权所有©2023美国气溶胶研究协会图形摘要
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引用次数: 1
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Aerosol Science and Technology
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