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Title: Investigation of pyruvic acid photolysis at the air-liquid interface as a source of aqueous secondary organic aerosols

Journal Article · · Science of the Total Environment
 [1];  [2];  [2];  [3]
  1. Shandong Normal Univ., Jinan (China)
  2. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
  3. Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Pyruvic acid (PA) is a ubiquitous 2-oxocarboxylic acid in the atmosphere. Its photochemical process at the air-liquid (a-l) interface has been suggested as an important source of aqueous secondary organic aerosols. Here, we investigated the photochemical reaction pathways of PA at the a-l interface using synchrotron-based vacuum ultraviolet single-photon ionization mass spectrometry (VUV SPI-MS) coupled with the System for Analysis at the Liquid Vacuum Interface (SALVI) microreactor. Results from mass spectral analysis and the determination of appearance energies (AEs) indicate that photolysis of PA can generate radicals, then they recombine with carboxylic acids and simple molecular oligomers. Furthermore, the preliminary products could form larger oligomers via radical reaction or esterification in the presence of hydroxyl and carboxyl functional groups. Mass spectral comparison shows that most photochemical reactions would complete within 4 h. The expanded photochemistry-driven reaction flowchart of PA is proposed based on the newly discovered products. Our results reveal that the interfacial PA photochemical reactions have different mechanisms from the bulk liquid due to the interfacial properties, such as molecular density, composition, and ion concentration. Our findings show that in situ mass spectral analysis with bright photon ionization is useful to elucidate the contribution of a-l interfacial reactions leading to aqSOA formation.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); USDOE Laboratory Directed Research and Development (LDRD) Program; Natural Science Foundation of Shandong Province
Grant/Contract Number:
AC05-00OR22725; AC02-05CH11231
OSTI ID:
2351091
Alternate ID(s):
OSTI ID: 2369846
Journal Information:
Science of the Total Environment, Journal Name: Science of the Total Environment Journal Issue: 1 Vol. 930; ISSN 0048-9697
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

References (59)

The toxicological analysis of secondary organic aerosol in human lung epithelial cells and macrophages journal June 2019
Making a hybrid microfluidic platform compatible for in situ imaging by vacuum-based techniques journal November 2011
Secondary organic aerosol formation in cloud droplets and aqueous particles (aqSOA): a review of laboratory, field and model studies journal January 2011
ATMOSPHERE: Enhanced: Air Pollution-Related Illness: Effects of Particles journal May 2005
From atoms to aerosols: probing clusters and nanoparticles with synchrotron based mass spectrometry and X-ray spectroscopy journal January 2020
Probing sulphur clusters in a microfluidic electrochemical cell with synchrotron-based photoionization mass spectrometry journal January 2020
Enhanced Acidity of Acetic and Pyruvic Acids on the Surface of Water journal July 2018
Liquid–Vapor Interface of Formic Acid Solutions in Salt Water: A Comparison of Macroscopic Surface Tension and Microscopic in Situ X-ray Photoelectron Spectroscopy Measurements journal August 2014
Kinetic Study of Gas-Phase Reactions of Pyruvic Acid with HO2 journal March 2021
Cross Photoreaction of Glyoxylic and Pyruvic Acids in Model Aqueous Aerosol journal July 2018
Volatility Change during Droplet Evaporation of Pyruvic Acid journal April 2020
Primary photodissociation mechanisms of pyruvic acid on S 1 : observation of methylhydroxycarbene and its chemical reaction in the gas phase journal January 2021
Evidence for Oligomer Formation in Clouds:  Reactions of Isoprene Oxidation Products journal August 2006
Detection of excited triplet species from photolysis of carbonyls: Direct evidence for single oxygen formation in atmospheric environment journal September 2022
Imaging liquids using microfluidic cells journal May 2013
Size-Dependent Sigmoidal Reaction Kinetics for Pyruvic Acid Condensation at the Air–Water Interface in Aqueous Microdroplets journal October 2023
Aqueous chemistry and its role in secondary organic aerosol (SOA) formation journal January 2010
Photochemistry of aqueous pyruvic acid journal July 2013
The decay of organic aerosols journal March 2005
Deciphering the aqueous chemistry of glyoxal oxidation with hydrogen peroxide using molecular imaging journal January 2017
Dark air–liquid interfacial chemistry of glyoxal and hydrogen peroxide journal August 2019
High secondary aerosol contribution to particulate pollution during haze events in China journal September 2014
Photochemical Kinetics of Pyruvic Acid in Aqueous Solution journal April 2014
Global modeling of SOA: the use of different mechanisms for aqueous-phase formation journal January 2014
Modeling Photosensitized Secondary Organic Aerosol Formation in Laboratory and Ambient Aerosols journal June 2017
CO2 Capture in Amine-Based Aqueous Solution: Role of the Gas-Solution Interface journal June 2011
Atmospheric Chemistry of Oxygenated Volatile Organic Compounds: Impacts on Air Quality and Climate journal February 2015
New Insights into Secondary Organic Aerosol Formation at the Air–Liquid Interface journal December 2020
Molecular investigation on the binding of Cd(II) by the binary mixtures of montmorillonite with two bacterial species journal October 2017
Light absorption and the photoformation of hydroxyl radical and singlet oxygen in fog waters journal September 2017
Aqueous Organic Chemistry in the Atmosphere: Sources and Chemical Processing of Organic Aerosols journal January 2015
Evolution of aqSOA from the Air–Liquid Interfacial Photochemistry of Glyoxal and Hydroxyl Radicals journal July 2019
Dissociative Photoionization of Glycerol and its Dimer Occurs Predominantly via a Ternary Hydrogen-Bridged Ion–Molecule Complex journal September 2013
Photochemical Synthesis of Oligomeric Amphiphiles from Alkyl Oxoacids in Aqueous Environments journal May 2017
Molecular characterization of atmospheric particulate organosulfates in a port environment using ultrahigh resolution mass spectrometry: Identification of traffic emissions journal October 2021
Photoemission from Liquid Aqueous Solutions journal April 2006
Secondary organic aerosol formation from semi- and intermediate-volatility organic compounds and glyoxal: Relevance of O/C as a tracer for aqueous multiphase chemistry: SOA FORMATION FROM S/IVOC AND GLYOXAL journal March 2013
Photoinduced Oligomerization of Aqueous Pyruvic Acid journal March 2006
ToF-SIMS characterization of glyoxal surface oxidation products by hydrogen peroxide: A comparison between dry and liquid samples: SIMS characterization of glyoxal surface oxidation by hydrogen peroxide journal November 2017
Photoelectron Spectroscopy Meets Aqueous Solution: Studies from a Vacuum Liquid Microjet journal February 2011
Laser Desorption Postionization Mass Spectrometry of Antibiotic-Treated Bacterial Biofilms Using Tunable Vacuum Ultraviolet Radiation journal September 2010
Vacuum Ultraviolet Photoionization of Complex Chemical Systems journal May 2016
Studying Interfacial Dark Reactions of Glyoxal and Hydrogen Peroxide Using Vacuum Ultraviolet Single Photon Ionization Mass Spectrometry journal March 2021
Enabling liquid vapor analysis using synchrotron VUV single photon ionization mass spectrometry with a microfluidic interface journal November 2018
Chemical Equilibria and Kinetics in Aqueous Solutions of Zymonic Acid journal December 2016
UHV and Ambient Pressure XPS: Potentials for Mg, MgO, and Mg(OH)2 Surface Analysis journal October 2016
Improving the Molecular Ion Signal Intensity for In Situ Liquid SIMS Analysis journal September 2016
In situ, in vivo, and in operando imaging and spectroscopy of liquids using microfluidics in vacuum journal June 2020
Does interfacial photochemistry play a role in the photolysis of pyruvic acid in water? journal October 2018
Irradiances of spectral lines in mercury pencil lamps journal January 1996
Development and initial evaluation of a dynamic species-resolved model for gas phase chemistry and size-resolved gas/particle partitioning associated with secondary organic aerosol formation journal January 2005
Photogeneration of Distant Radical Pairs in Aqueous Pyruvic Acid Glasses journal January 2006
Investigation of solid/vapor interfaces using ambient pressure X-ray photoelectron spectroscopy journal January 2013
Mechanistic Description of Photochemical Oligomer Formation from Aqueous Pyruvic Acid journal May 2017
Development of novel correlative light and electron microscopy linkage system using silicon nitride film journal January 2019
Spatial Distribution of Nitrate and Nitrite Anions at the Liquid/Vapor Interface of Aqueous Solutions journal June 2009
Analytical advances to study the air – water interfacial chemistry in the atmosphere journal December 2022
Multiphase Photochemistry of Pyruvic Acid under Atmospheric Conditions journal April 2017
Particle Phase Acidity and Oligomer Formation in Secondary Organic Aerosol journal December 2004