High Pressure Inside Nanometer-Sized Particles Influences the Rate and Products of Chemical Reactions,Environmental Science & Technology

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High Pressure Inside Nanometer-Sized Particles Influences the Rate and Products of Chemical Reactions
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2021-06-01 , DOI: 10.1021/acs.est.0c07386
Matthieu Riva ₁ , Jianfeng Sun _{1,

2} , V Faye McNeill ₃ , Charline Ragon ₁ , Sebastien Perrier ₁ , Yinon Rudich ₄ , Sergey A Nizkorodov ₅ , Jianmin Chen ₂ , Frédéric Caupin ₆ , Thorsten Hoffmann ₇ , Christian George ₁

Affiliation

The composition of organic aerosol has a pivotal influence on aerosol properties such as toxicity and cloud droplet formation capability, which could affect both climate and air quality. However, a comprehensive and fundamental understanding of the chemical and physical processes that occur in nanometer-sized atmospheric particles remains a challenge that severely limits the quantification and predictive capabilities of aerosol formation pathways. Here, we investigated the effects of a fundamental and hitherto unconsidered physical property of nanoparticles—the Laplace pressure. By studying the reaction of glyoxal with ammonium sulfate, both ubiquitous and important atmospheric constituents, we show that high pressure can significantly affect the chemical processes that occur in atmospheric ultrafine particles (i.e., particles < 100 nm). Using high-resolution mass spectrometry and UV–vis spectroscopy, we demonstrated that the formation of reaction products is strongly (i.e., up to a factor of 2) slowed down under high pressures typical of atmospheric nanoparticles. A size-dependent relative rate constant is determined and numerical simulations illustrate the reduction in the production of the main glyoxal reaction products. These results established that the high pressure inside nanometer-sized aerosols must be considered as a key property that significantly impacts chemical processes that govern atmospheric aerosol growth and evolution.

中文翻译：

纳米级粒子内部的高压影响化学反应的速率和产物

有机气溶胶的组成对气溶胶的毒性和云滴形成能力等性质有关键影响，这可能会影响气候和空气质量。然而，对纳米级大气粒子中发生的化学和物理过程的全面和基本的理解仍然是一个挑战，严重限制了气溶胶形成途径的量化和预测能力。在这里，我们研究了纳米粒子的一个基本的和迄今为止未被考虑的物理特性——拉普拉斯压力的影响。通过研究乙二醛与硫酸铵（普遍存在且重要的大气成分）的反应，我们表明高压可以显着影响大气超细颗粒（即颗粒 < 100 nm）中发生的化学过程。使用高分辨率质谱和紫外-可见光谱，我们证明了反应产物的形成在大气纳米粒子典型的高压下强烈（即高达 2 倍）减慢。确定了与尺寸相关的相对速率常数，并且数值模拟说明了主要乙二醛反应产物的产量减少。这些结果表明，纳米级气溶胶内部的高压必须被视为一个关键特性，它显着影响控制大气气溶胶生长和演化的化学过程。确定了与尺寸相关的相对速率常数，并且数值模拟说明了主要乙二醛反应产物的产量减少。这些结果表明，纳米级气溶胶内部的高压必须被视为一个关键特性，它显着影响控制大气气溶胶生长和演化的化学过程。确定了与尺寸相关的相对速率常数，并且数值模拟说明了主要乙二醛反应产物的产量减少。这些结果表明，纳米级气溶胶内部的高压必须被视为一个关键特性，它显着影响控制大气气溶胶生长和演化的化学过程。

更新日期：2021-06-15

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