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Organic Aerosol Dynamics: Molecular Interactions, Single Particles and Modest Driving Forces

有机气溶胶动力学：分子相互作用、单粒子和适度的驱动力

基本信息

批准号：
1807530
负责人：
Neil Donahue
金额：
$ 40万
依托单位：
Carnegie-Mellon University
依托单位国家：
美国
项目类别：
Standard Grant
财政年份：
2018
资助国家：
美国
起止时间：
2018-08-01 至 2021-07-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1807530&HistoricalAwards=false
关键词：
Organic Aerosol Dynamics Molecular Interactions

项目摘要

Fine particles play a key role in atmospheric chemistry, and effect human health and weather. The physical and chemical properties of fine particles are critical in controlling their behavior. The properties of these particles are significantly different from liquids or solids. Typical particles are about 300 nanometers in diameter and contain roughly 10 million individual molecules. Well over half of those molecules are organic (carbon containing) compounds, and even a single particle often contains hundreds of thousands of different organic molecules, most of which have never been isolated or synthesized by chemists. These organic molecules stick to the tiny particles rather than letting go of the particle and floating (volatilizing) into the air. Some of the organic compounds resemble asphalt or complex sugars. This research advances fundamental understanding of how combustion processes and products related to energy production may influence human health. Professor Neil Donahue and his graduate students at Carnegie Mellon University study the behavior of a number of model systems using sophisticated mass spectrometers that can measure the composition of individual 300 nm particles along with complementary chemical ionization mass spectrometers that can measure individual molecules in the gas and particle phases. They generate organic particles mimicking those found in the atmosphere with progressively higher degrees of oxidation to see if the particles become more viscous in a way that matters - by directly testing if semi-volatile organics can diffuse into the particles and whether two initially distinct populations of particles with semi-volatile constituents evolve toward each other because of mixing. The researchers conduct these experiments over a wide range of relative humidity conditions as humidity varies widely in the atmosphere and because wet particles are known to be much less viscous and more diffusive. Via a collaboration with colleagues at Northwestern University, they use synthesized molecules containing the stable carbon isotope, 13C, to cleanly separate molecules from different particle populations using mass spectrometry. The project prepares doctoral students for a research career. Professor Donahue is an ambassador in the Science and Engineering Ambassadors Program founded by the National Academies. He brings a focus on the coupling between energy use and environmental health issues.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

细颗粒物在大气化学中起着重要作用，影响着人类健康和天气。细颗粒的物理和化学性质对控制其行为至关重要。这些颗粒的性质与液体或固体有很大的不同。典型的粒子直径约为300纳米，含有大约1000万个单个分子。这些分子中有一半以上是有机（含碳）化合物，即使是一个单一的颗粒也往往包含数十万种不同的有机分子，其中大多数从未被化学家分离或合成。这些有机分子粘在微小的颗粒上，而不是释放颗粒并漂浮（挥发）到空气中。一些有机化合物类似于沥青或复合糖。这项研究推进了对与能源生产有关的燃烧过程和产物如何影响人类健康的基本理解。卡内基梅隆大学的Neil Donahue教授和他的研究生使用复杂的质谱仪研究了许多模型系统的行为，这些质谱仪可以测量单个300 nm颗粒的组成，沿着补充化学电离质谱仪可以测量气相和颗粒相的单个分子。它们产生的有机颗粒模仿大气中发现的那些，氧化程度逐渐提高，以观察颗粒是否以重要的方式变得更加粘稠-通过直接测试半挥发性有机物是否可以扩散到颗粒中，以及两种最初不同的颗粒群是否具有半挥发性成分由于混合而相互进化。研究人员在大范围的相对湿度条件下进行这些实验，因为大气中的湿度变化很大，而且已知湿颗粒的粘性要小得多，扩散性更强。通过与西北大学的同事合作，他们使用含有稳定碳同位素13 C的合成分子，使用质谱法从不同的粒子群中干净地分离分子。该项目为博士生的研究生涯做好准备。Donahue教授是美国国家科学院创办的科学与工程大使计划的大使。该奖项反映了NSF的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

项目成果

期刊论文数量（7）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

Single particle measurements of mixing between mimics for biomass burning and aged secondary organic aerosols

生物质燃烧模拟物与老化二次有机气溶胶之间混合的单粒子测量

DOI：
10.1039/d2ea00017b
发表时间：
2022
期刊：
Environmental Science: Atmospheres
影响因子：
0
作者：
Habib, Luke;Donahue, Neil
通讯作者：
Donahue, Neil

Moving beyond Fine Particle Mass: High-Spatial Resolution Exposure to Source-Resolved Atmospheric Particle Number and Chemical Mixing State

DOI：
10.1289/ehp5311
发表时间：
2020-01-01
期刊：
ENVIRONMENTAL HEALTH PERSPECTIVES
影响因子：
10.4
作者：
Ye, Qing;Li, Hugh Z.;Presto, Albert A.
通讯作者：
Presto, Albert A.

Gas-Phase Organic Oxidation Chemistry and Atmospheric Particles

气相有机氧化化学和大气颗粒

DOI：
10.1142/9789813271838_0004
发表时间：
2019
期刊：
Advances in atmospheric chemistry
影响因子：
0
作者：
Donahue, Neil M.;Chuang, Wayne;Schervish, Meredith
通讯作者：
Schervish, Meredith

Using Ionic Liquids To Study the Migration of Semivolatile Organic Vapors in Smog Chamber Experiments

利用离子液体研究烟雾室实验中半挥发性有机蒸气的迁移

DOI：
10.1021/acs.jpca.9b02847
发表时间：
2019
期刊：
The Journal of Physical Chemistry A
影响因子：
0
作者：
Ye, Qing;Sullivan, Ryan C.;Donahue, Neil M.
通讯作者：
Donahue, Neil M.

Molecular Composition of Oxygenated Organic Molecules and Their Contributions to Organic Aerosol in Beijing

含氧有机分子的分子组成及其对北京有机气溶胶的贡献

DOI：
10.1021/acs.est.1c05191
发表时间：
2022
期刊：
Environ. Sci. Technol.
影响因子：
0
作者：
Yonghong Wang;Petri Clusius;Chao Yan;Kaspar Dällenbach;Rujing Yin;Mingyi Wang;Xu-Cheng He;Biwu Chu;Yiqun Lu;Lubna Dada;Juha Kangasluoma;Pekka Rantala;Chenjuan Deng;Zhuohui Lin;Weigang Wang;Lei Yao;Xiaolong Fan;Wei Du;Jing Cai;Liine Heikkinen;Yee Jun Tham
通讯作者：
Yee Jun Tham