Formation of highly oxidized multifunctional compounds: autoxidation of peroxy radicals formed in the ozonolysis of alkenes – deduced from structure–product relationships DOI Creative Commons
Thomas F. Mentel,

Monika Springer,

Mikael Ehn

et al.

Atmospheric chemistry and physics, Journal Year: 2015, Volume and Issue: 15(12), P. 6745 - 6765

Published: June 18, 2015

Abstract. It has been postulated that secondary organic particulate matter plays a pivotal role in the early growth of newly formed particles forest areas. The recently detected class extremely low volatile compounds (ELVOC) provides missing vapors and possibly contributes significant fraction to atmospheric SOA (secondary aerosol). sequential rearrangement peroxy radicals subsequent O2 addition results ELVOC which are highly oxidized multifunctional molecules (HOM). Key for efficiency such HOM particle is their formation induced by one attack oxidant (here O3), followed an autoxidation process involving molecular oxygen. Similar mechanisms were observed predicted quantum mechanical calculations e.g., isoprene. To assess importance therewith potential generality, it crucial understand pathway HOM. elucidate path as well necessary sufficient structural prerequisites we studied homologous series cycloalkenes comparison two monoterpenes. We able directly observe with 8 or 10 O atoms Atmospheric Pressure interface High Resolution Time Flight Mass Spectrometer (APi-TOF-MS) equipped NO3−-chemical ionization (CI) source. In case O3 acting oxidant, starting radical on so-called vinylhydroperoxide path. termination reactions other radicals, including dimerization, allowed analyzing mass spectra narrowing down likely As consequence, propose percarboxylic acids, carbonyl, hydroperoxy, hydroxy groups arising from steps. figured aldehyde facilitate initial simple like cycloalkenes, was limited both terminal C further respective α positions. more complex containing tertiary H small, constrained rings, even higher oxidation degrees possible, either shift atom initialization ring-opening reactions.

Language: Английский

Elucidating severe urban haze formation in China DOI Open Access
Song Guo, Min Hu, Misti Levy Zamora

et al.

Proceedings of the National Academy of Sciences, Journal Year: 2014, Volume and Issue: 111(49), P. 17373 - 17378

Published: Nov. 24, 2014

Significance We illustrate the similarity and difference in particulate matter (PM) formation between Beijing other world regions. The periodic cycle of PM events is regulated by meteorological conditions. While particle chemical compositions are similar to those commonly measured worldwide, efficient nucleation growth over an extended period distinctive from aerosol typically observed global areas. Gaseous emissions volatile organic compounds nitrogen oxides urban transportation sulfur dioxide regional industry responsible for large secondary formation, while primary transport insignificant. Reductions precursor gases essential mediate severe haze pollution China.

Language: Английский

Citations

1744

Formation of Urban Fine Particulate Matter DOI
Renyi Zhang,

Gehui Wang,

Song Guo

et al.

Chemical Reviews, Journal Year: 2015, Volume and Issue: 115(10), P. 3803 - 3855

Published: May 5, 2015

ADVERTISEMENT RETURN TO ISSUEPREVReviewNEXTFormation of Urban Fine Particulate MatterRenyi Zhang*†§, Gehui Wang†∥, Song Guo†§, Misti L. Zamora†, Qi Ying‡, Yun Lin†, Weigang Wang†⊥, Min Hu§, and Yuan Wang#View Author Information† †Departments Atmospheric Sciences Chemistry ‡Department Civil Engineering, Texas A&M University, College Station, 77843, United States§ State Key Joint Laboratory Environmental Simulation Pollution Control, Peking Beijing 100871, People's Republic China⊥ ∥Key Aerosol Physics Chemistry, Loess Quaternary Geology, Institute Earth Environment, ⊥State for Structural Unstable Stable Species, National Molecular (BNLMS), Chinese Academy Sciences, 100864, China# Jet Propulsion Laboratory, California Technology, Pasadena, 91125, States*E-mail: [email protected]Cite this: Chem. Rev. 2015, 115, 10, 3803–3855Publication Date (Web):May 5, 2015Publication History Received2 February 2015Published online5 May inissue 27 2015https://pubs.acs.org/doi/10.1021/acs.chemrev.5b00067https://doi.org/10.1021/acs.chemrev.5b00067review-articleACS PublicationsCopyright © 2015 American Chemical SocietyRequest reuse permissionsArticle Views17488Altmetric-Citations927LEARN ABOUT THESE METRICSArticle Views are the COUNTER-compliant sum full text article downloads since November 2008 (both PDF HTML) across all institutions individuals. These metrics regularly updated to reflect usage leading up last few days.Citations number other articles citing this article, calculated by Crossref daily. Find more information about citation counts.The Altmetric Attention Score is a quantitative measure attention that research has received online. Clicking on donut icon will load page at altmetric.com with additional details score social media presence given article. how calculated. Share Add toView InAdd Full Text ReferenceAdd Description ExportRISCitationCitation abstractCitation referencesMore Options onFacebookTwitterWechatLinked InRedditEmail Other access optionsGet e-Alertsclose SUBJECTS:Aerosols,Anions,Nanoparticles,Particulate matter,Volatile organic compounds Get e-Alerts

Language: Английский

Citations

1322

Highly Oxygenated Organic Molecules (HOM) from Gas-Phase Autoxidation Involving Peroxy Radicals: A Key Contributor to Atmospheric Aerosol DOI Creative Commons
Federico Bianchi, Theo Kurtén, Matthieu Riva

et al.

Chemical Reviews, Journal Year: 2019, Volume and Issue: 119(6), P. 3472 - 3509

Published: Feb. 25, 2019

Highly oxygenated organic molecules (HOM) are formed in the atmosphere via autoxidation involving peroxy radicals arising from volatile compounds (VOC). HOM condense on pre-existing particles and can be involved new particle formation. thus contribute to formation of secondary aerosol (SOA), a significant ubiquitous component atmospheric known affect Earth's radiation balance. were discovered only very recently, but interest these has grown rapidly. In this Review, we define describe currently available techniques for their identification/quantification, followed by summary current knowledge mechanisms physicochemical properties. A main aim is provide common frame quite fragmented literature studies. Finally, highlight existing gaps our understanding suggest directions future research.

Language: Английский

Citations

990

Trees, forests and water: Cool insights for a hot world DOI Creative Commons
David Ellison, Cindy E. Morris, Bruno Locatelli

et al.

Global Environmental Change, Journal Year: 2017, Volume and Issue: 43, P. 51 - 61

Published: Feb. 9, 2017

Forest-driven water and energy cycles are poorly integrated into regional, national, continental global decision-making on climate change adaptation, mitigation, land use management. This constrains humanity’s ability to protect our planet’s life-sustaining functions. The substantial body of research we review reveals that forest, interactions provide the foundations for carbon storage, cooling terrestrial surfaces distributing resources. Forests trees must be recognized as prime regulators within water, cycles. If these functions ignored, planners will unable assess, adapt or mitigate impacts changing cover climate. Our call action targets a reversal paradigms, from carbon-centric model one treats hydrologic climate-cooling effects forests first order priority. For reasons sustainability, storage remain secondary, though valuable, by-product. tree at local, regional scales offer benefits demand wider recognition. forest- tree-centered insights analyze knowledge-base improving plans, policies actions. understanding how influence has important implications, both structure planning, management governance institutions, well might used improve adaptation mitigation efforts.

Language: Английский

Citations

960

Recent advances in understanding secondary organic aerosol: Implications for global climate forcing DOI Creative Commons
Manish Shrivastava, Christopher D. Cappa, Jiwen Fan

et al.

Reviews of Geophysics, Journal Year: 2017, Volume and Issue: 55(2), P. 509 - 559

Published: May 18, 2017

Abstract Anthropogenic emissions and land use changes have modified atmospheric aerosol concentrations size distributions over time. Understanding preindustrial conditions in organic due to anthropogenic activities is important because these features (1) influence estimates of radiative forcing (2) can confound the historical response climate increases greenhouse gases. Secondary (SOA), formed atmosphere by oxidation gases, represents a major fraction global submicron‐sized aerosol. Over past decade, significant advances understanding SOA properties formation mechanisms occurred through measurements, yet current models typically do not comprehensively include all processes. This review summarizes some developments during decade formation. We highlight importance processes that growth particles sizes relevant for clouds forcing, including extremely low volatility organics gas phase, acid‐catalyzed multiphase chemistry isoprene epoxydiols, particle‐phase oligomerization, physical such as viscosity. Several highlighted this are complex interdependent nonlinear effects on properties, formation, evolution SOA. Current neglect complexity nonlinearity thus less likely accurately predict project future sensitivity Efforts also needed rank most influential process‐related interactions, so be represented chemistry‐climate models.

Language: Английский

Citations

933

Particulate matter, air quality and climate: lessons learned and future needs DOI Creative Commons
S. Fuzzi, Urs Baltensperger, K. S. Carslaw

et al.

Atmospheric chemistry and physics, Journal Year: 2015, Volume and Issue: 15(14), P. 8217 - 8299

Published: July 24, 2015

Abstract. The literature on atmospheric particulate matter (PM), or aerosol, has increased enormously over the last 2 decades and amounts now to some 1500–2000 papers per year in refereed literature. This is part due enormous advances measurement technologies, which have allowed for an increasingly accurate understanding of chemical composition physical properties particles their processes atmosphere. growing scientific interest aerosol high importance environmental policy. In fact, constitutes one most challenging problems both air quality climate change policies. this context, paper reviews recent results within sciences policy needs, driven much increase monitoring mechanistic research decades. synthesis reveals many new developments science underpinning climate–aerosol interactions effects PM human health environment. However, while airborne responsible globally important influences premature mortality, we still do not know relative different components these effects. Likewise, magnitude overall remains highly uncertain. Despite uncertainty there are things that could be done mitigate local global PM. Recent analyses shown reducing black carbon (BC) emissions, using known control measures, would reduce warming delay time when anthropogenic temperature exceed °C. cost-effective measures ammonia, agricultural precursor gas secondary inorganic aerosols (SIA), regional eutrophication concentrations large areas Europe, China USA. Thus, environment population. A prioritized list actions full range currently undeliverable shortcomings knowledge science; among shortcomings, roles sources response land use remaining century prominent. any case, evidence from strongly advocates integrated approach

Language: Английский

Citations

843

The role of low-volatility organic compounds in initial particle growth in the atmosphere DOI Creative Commons
Jasmin Tröstl,

Wayne K. Chuang,

Hamish Gordon

et al.

Nature, Journal Year: 2016, Volume and Issue: 533(7604), P. 527 - 531

Published: May 25, 2016

Abstract About half of present-day cloud condensation nuclei originate from atmospheric nucleation, frequently appearing as a burst new particles near midday 1 . Atmospheric observations show that the growth rate often accelerates when diameter is between one and ten nanometres 2,3 In this critical size range, are most likely to be lost by coagulation with pre-existing 4 , thereby failing form typically 50 100 across. Sulfuric acid vapour involved in nucleation but too scarce explain subsequent 5,6 leaving organic vapours plausible alternative, at least planetary boundary layer 7,8,9,10 Although recent studies 11,12,13 predict low-volatility contribute during initial growth, direct evidence has been lacking. The accelerating may result increased photolytic production condensable species afternoon 2 presence possible Kelvin (curvature) effect, which inhibits on smallest (the nano-Köhler theory) 2,14 so far remained ambiguous. Here we present experiments performed large chamber under conditions investigate role nucleated absence inorganic acids bases such sulfuric or ammonia amines, respectively. Using data same set experiments, it shown 15 alone can drive nucleation. We focus find have extremely low volatilities (saturation concentration less than 10 −4.5 micrograms per cubic metre). As increase barrier falls, primarily due more abundant slightly higher volatility concentrations −0.5 particle model quantitatively reproduces our measurements. Furthermore, implement parameterization first steps global aerosol change substantially response, is, up cent comparison previously assumed parameterizations.

Language: Английский

Citations

832

Ion-induced nucleation of pure biogenic particles DOI Creative Commons
J. Kirkby, Jonathan Duplissy,

Kamalika Sengupta

et al.

Nature, Journal Year: 2016, Volume and Issue: 533(7604), P. 521 - 526

Published: May 25, 2016

Abstract Atmospheric aerosols and their effect on clouds are thought to be important for anthropogenic radiative forcing of the climate, yet remain poorly understood 1 . Globally, around half cloud condensation nuclei originate from nucleation atmospheric vapours 2 It is that sulfuric acid essential initiate most particle formation in atmosphere 3,4 , ions have a relatively minor role 5 Some laboratory studies, however, reported organic without intentional addition acid, although contamination could not excluded 6,7 Here we present evidence aerosol particles highly oxidized biogenic absence large chamber under conditions. The oxygenated molecules (HOMs) produced by ozonolysis α-pinene. We find Galactic cosmic rays increase rate one two orders magnitude compared with neutral nucleation. Our experimental findings supported quantum chemical calculations cluster binding energies representative HOMs. Ion-induced pure constitutes potentially widespread source terrestrial environments low pollution.

Language: Английский

Citations

760

Atmospheric new particle formation from sulfuric acid and amines in a Chinese megacity DOI Open Access
Lei Yao, Olga Garmаsh, Federico Bianchi

et al.

Science, Journal Year: 2018, Volume and Issue: 361(6399), P. 278 - 281

Published: July 19, 2018

Atmospheric new particle formation (NPF) is an important global phenomenon that nevertheless sensitive to ambient conditions. According both observation and theoretical arguments, NPF usually requires a relatively high sulfuric acid (H2SO4) concentration promote the of particles low preexisting aerosol loading minimize sink particles. We investigated in Shanghai were able observe precursor vapors initial clusters at molecular level megacity. High rates observed coincide with several familiar markers suggestive H2SO4-dimethylamine (DMA)-water (H2O) nucleation, including dimers H2SO4-DMA clusters. In cluster kinetics simulation, was enough explain growth ~3 nanometers under very condensation sink, whereas subsequent higher rate beyond this size believed result from added contribution condensing organic species. These findings will help understanding urban its air quality climate effects, as well formulating policies mitigate secondary China.

Language: Английский

Citations

660

The Molecular Identification of Organic Compounds in the Atmosphere: State of the Art and Challenges DOI
Barbara Nozière, Markus Kalberer, Magda Claeys

et al.

Chemical Reviews, Journal Year: 2015, Volume and Issue: 115(10), P. 3919 - 3983

Published: Feb. 3, 2015

ADVERTISEMENT RETURN TO ISSUEPREVReviewNEXTThe Molecular Identification of Organic Compounds in the Atmosphere: State Art and ChallengesBarbara Nozière*†, Markus Kalberer*‡, Magda Claeys*§, James Allan∥, Barbara D'Anna†, Stefano Decesari⊥, Emanuela Finessi#, Marianne Glasius∇, Irena Grgić○, Jacqueline F. Hamilton#, Thorsten Hoffmann◆, Yoshiteru Iinuma¶, Mohammed Jaoui△, Ariane Kahnt§, Christopher J. Kampf▲, Ivan Kourtchev‡, Willy Maenhaut§□, Nicholas Marsden∥, Sanna Saarikoski■, Jürgen Schnelle-Kreis◇, Jason D. Surratt▼, Sönke Szidat☆, Rafal Szmigielski★, Armin Wisthaler⬡View Author Information† Ircelyon/CNRS Université Lyon 1, 69626 Villeurbanne Cedex, France‡ University Cambridge, Cambridge CB2 1EW, United Kingdom§ Antwerp, 2000 Belgium∥ The Manchester & National Centre for Atmospheric Science, M13 9PL, Kingdom⊥ Istituto ISAC - C.N.R., I-40129 Bologna, Italy# York, York YO10 5DD, Kingdom∇ Aarhus, 8000 Aarhus C, Denmark○ Institute Chemistry, 1000 Ljubljana, Slovenia◆ Johannes Gutenberg-Universität, 55122 Mainz, Germany¶ Leibniz-Institut für Troposphärenforschung, 04318 Leipzig, Germany△ Alion Science Technology, McLean, Virginia 22102, States▲ Max Planck 55128 Germany□ Ghent University, 9000 Gent, Belgium■ Finnish Meteorological Institute, FI-00101 Helsinki, Finland◇ Helmholtz Zentrum München, D-85764 Neuherberg, Germany▼ North Carolina at Chapel Hill, 27599, States☆ Bern, 3012 Switzerland★ Physical Chemistry PAS, Warsaw 01-224, Poland⬡ Oslo, 0316 Norway*E-mail: [email protected]*E-mail: protected]Cite this: Chem. Rev. 2015, 115, 10, 3919–3983Publication Date (Web):February 3, 2015Publication History Received1 July 2014Published online3 February 2015Published inissue 27 May 2015https://pubs.acs.org/doi/10.1021/cr5003485https://doi.org/10.1021/cr5003485review-articleACS PublicationsCopyright © 2015 American Chemical SocietyRequest reuse permissionsArticle Views12686Altmetric-Citations384LEARN ABOUT THESE METRICSArticle Views are COUNTER-compliant sum full text article downloads since November 2008 (both PDF HTML) across all institutions individuals. These metrics regularly updated to reflect usage leading up last few days.Citations number other articles citing this article, calculated by Crossref daily. Find more information about citation counts.The Altmetric Attention Score is a quantitative measure attention that research has received online. Clicking on donut icon will load page altmetric.com with additional details score social media presence given article. how calculated. Share Add toView InAdd Full Text ReferenceAdd Description ExportRISCitationCitation abstractCitation referencesMore Options onFacebookTwitterWechatLinked InRedditEmail Other access optionsGet e-Alertsclose SUBJECTS:Aerosols,Chromatography,Mathematical methods,Organic compounds,Redox reactions Get e-Alerts

Language: Английский

Citations

634