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DOI | 10.1073/pnas.1720488115 |
Aerosol microdroplets exhibit a stable pH gradient | |
Wei, Haoran1,2,3; Vejerano, Eric P.1,2,3,4; Leng, Weinan1,2,3; Huang, Qishen1,2,3; Willner, Marjorie R.1,2,3; Marr, Linsey C.1,2,3; Vikesland, Peter J.1,2,3 | |
2018-07-10 | |
发表期刊 | PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA |
ISSN | 0027-8424 |
出版年 | 2018 |
卷号 | 115期号:28页码:7272-7277 |
文章类型 | Article |
语种 | 英语 |
国家 | USA |
英文摘要 | Suspended aqueous aerosol droplets (< 50 mu m) are microreactors for many important atmospheric reactions. In droplets and other aquatic environments, pH is arguably the key parameter dictating chemical and biological processes. The nature of the droplet air/water interface has the potential to significantly alter droplet pH relative to bulk water. Historically, it has been challenging to measure the pH of individual droplets because of their inaccessibility to conventional pH probes. In this study, we scanned droplets containing 4-mercaptobenzoic acid-functionalized gold nanoparticle pH nanoprobes by 2D and 3D laser confocal Raman microscopy. Using surface-enhanced Raman scattering, we acquired the pH distribution inside approximately 20-mu m-diameter phosphate-buffered aerosol droplets and found that the pH in the core of a droplet is higher than that of bulk solution by up to 3.6 pH units. This finding suggests the accumulation of protons at the air/water interface and is consistent with recent thermodynamic model results. The existence of this pH shift was corroborated by the observation that a catalytic reaction that occurs only under basic conditions (i.e., dimerization of 4-aminothiophenol to produce dimercaptoazobenzene) occurs within the high pH core of a droplet, but not in bulk solution. Our nanoparticle probe enables pH quantification through the cross-section of an aerosol droplet, revealing a spatial gradient that has implications for acid-base-catalyzed atmospheric chemistry. |
英文关键词 | aerosol droplet pH interface SERS |
领域 | 地球科学 ; 气候变化 ; 资源环境 |
收录类别 | SCI-E |
WOS记录号 | WOS:000438050900058 |
WOS关键词 | ENHANCED RAMAN-SPECTROSCOPY ; CATALYZED REACTIVE UPTAKE ; MARINE BOUNDARY-LAYER ; AIR-WATER-INTERFACE ; ORGANIC AEROSOL ; AIR/WATER INTERFACE ; ATMOSPHERIC AEROSOL ; SURFACE ; PHASE ; NANOPARTICLES |
WOS类目 | Multidisciplinary Sciences |
WOS研究方向 | Science & Technology - Other Topics |
URL | 查看原文 |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://119.78.100.173/C666/handle/2XK7JSWQ/204950 |
专题 | 地球科学 资源环境科学 气候变化 |
作者单位 | 1.Virginia Tech, Dept Civil & Environm Engn, Blacksburg, VA 24061 USA; 2.Virginia Tech Inst Crit Technol & Appl Sci, Sustainable Nanotechnol Ctr, Blacksburg, VA 24061 USA; 3.Duke Univ, Ctr Environm Implicat Nanotechnol, Durham, NC 27708 USA; 4.Univ South Carolina, Arnold Sch Publ Hlth, Columbia, SC 29208 USA |
推荐引用方式 GB/T 7714 | Wei, Haoran,Vejerano, Eric P.,Leng, Weinan,et al. Aerosol microdroplets exhibit a stable pH gradient[J]. PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA,2018,115(28):7272-7277. |
APA | Wei, Haoran.,Vejerano, Eric P..,Leng, Weinan.,Huang, Qishen.,Willner, Marjorie R..,...&Vikesland, Peter J..(2018).Aerosol microdroplets exhibit a stable pH gradient.PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA,115(28),7272-7277. |
MLA | Wei, Haoran,et al."Aerosol microdroplets exhibit a stable pH gradient".PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA 115.28(2018):7272-7277. |
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