Abundant Nitrogenous Secondary Organic Aerosol Formation Accelerated by Cloud Processing

Overview

Journal iScience

Publisher Cell Press

Date 2023 Nov 29

PMID 38026147

Authors

Zhe Liu

Bao Zhu

Chao Zhu

Ting Ruan

Jiarong Li

Hui Chen

Qing Li

Xiaofei Wang

Lin Wang

Yujing Mu

Jeffrey Collett Jr

Christian George

Yan Wang

Xinfeng Wang

Jixin Su

Shaocai Yu

Abdewahid Mellouki

Jianmin Chen

Guibin Jiang

Affiliations

Soon will be listed here.

Abstract

Nitrogenous organic (CHON), crucial for secondary organic aerosol (SOA), forms through poorly studied mechanisms in clouds. Our study explores CHON transformation during cloud processes (CPs). These processes play a vital role in enhancing the variety of CHONs, leading to the formation of CHONs with oxygen atom counts ranging from 1 to 10 and double bond equivalent (DBE) values spanning from 2 to 10. We proposed that the CHONs formed during CPs are formed through aqueous phase reactions with CHO compound precursors via nucleophilic attacks by NH. This scheme can be account for roughly three-quarters of the CHONs by number in cloud water, and near two-thirds of all CHONs are formed through reactions between NH and carbonyl-containing biogenic volatile organic compound (BVOC) ozonolysis intermediates. This study provides the first insights into the evolution of CHONs during CPs and reveals the significant roles of CPs in the formation of CHONs.

References

Mohr C, Thornton J, Heitto A, Lopez-Hilfiker F, Lutz A, Riipinen I . Molecular identification of organic vapors driving atmospheric nanoparticle growth. Nat Commun. 2019; 10(1):4442. PMC: 6769005. DOI: 10.1038/s41467-019-12473-2. View

Lin P, Rincon A, Kalberer M, Yu J . Elemental composition of HULIS in the Pearl River Delta Region, China: results inferred from positive and negative electrospray high resolution mass spectrometric data. Environ Sci Technol. 2012; 46(14):7454-62. DOI: 10.1021/es300285d. View

Lee A, Zhao R, Li R, Liggio J, Li S, Abbatt J . Formation of light absorbing organo-nitrogen species from evaporation of droplets containing glyoxal and ammonium sulfate. Environ Sci Technol. 2013; 47(22):12819-26. DOI: 10.1021/es402687w. View

Hao L, Romakkaniemi S, Kortelainen A, Jaatinen A, Portin H, Miettinen P . Aerosol chemical composition in cloud events by high resolution time-of-flight aerosol mass spectrometry. Environ Sci Technol. 2013; 47(6):2645-53. DOI: 10.1021/es302889w. View

Bianco A, Deguillaume L, Vaitilingom M, Nicol E, Baray J, Chaumerliac N . Molecular Characterization of Cloud Water Samples Collected at the Puy de Dôme (France) by Fourier Transform Ion Cyclotron Resonance Mass Spectrometry. Environ Sci Technol. 2018; 52(18):10275-10285. DOI: 10.1021/acs.est.8b01964. View

Wang X, Gao S, Yang X, Chen H, Chen J, Zhuang G . Evidence for high molecular weight nitrogen-containing organic salts in urban aerosols. Environ Sci Technol. 2010; 44(12):4441-6. DOI: 10.1021/es1001117. View

Woo J, Kim D, Schwier A, Li R, McNeill V . Aqueous aerosol SOA formation: impact on aerosol physical properties. Faraday Discuss. 2014; 165:357-67. DOI: 10.1039/c3fd00032j. View

Seinfeld J, Bretherton C, Carslaw K, Coe H, DeMott P, Dunlea E . Improving our fundamental understanding of the role of aerosol-cloud interactions in the climate system. Proc Natl Acad Sci U S A. 2016; 113(21):5781-90. PMC: 4889348. DOI: 10.1073/pnas.1514043113. View

De Haan D, Hawkins L, Kononenko J, Turley J, Corrigan A, Tolbert M . Formation of nitrogen-containing oligomers by methylglyoxal and amines in simulated evaporating cloud droplets. Environ Sci Technol. 2010; 45(3):984-91. DOI: 10.1021/es102933x. View

10.

Zhu Y, Yang L, Kawamura K, Chen J, Ono K, Wang X . Contributions and source identification of biogenic and anthropogenic hydrocarbons to secondary organic aerosols at Mt. Tai in 2014. Environ Pollut. 2016; 220(Pt B):863-872. DOI: 10.1016/j.envpol.2016.10.070. View

11.

An Z, Huang R, Zhang R, Tie X, Li G, Cao J . Severe haze in northern China: A synergy of anthropogenic emissions and atmospheric processes. Proc Natl Acad Sci U S A. 2019; 116(18):8657-8666. PMC: 6500134. DOI: 10.1073/pnas.1900125116. View

12.

Liu Y, Ma Q, He H . Heterogeneous uptake of amines by citric acid and humic acid. Environ Sci Technol. 2012; 46(20):11112-8. DOI: 10.1021/es302414v. View

13.

Marrero-Ortiz W, Hu M, Du Z, Ji Y, Wang Y, Guo S . Formation and Optical Properties of Brown Carbon from Small α-Dicarbonyls and Amines. Environ Sci Technol. 2018; 53(1):117-126. DOI: 10.1021/acs.est.8b03995. View

14.

Zhang D, Zhang R . Ozonolysis of alpha-pinene and beta-pinene: kinetics and mechanism. J Chem Phys. 2005; 122(11):114308. DOI: 10.1063/1.1862616. View

15.

Mazzoleni L, Ehrmann B, Shen X, Marshall A, Collett Jr J . Water-soluble atmospheric organic matter in fog: exact masses and chemical formula identification by ultrahigh-resolution fourier transform ion cyclotron resonance mass spectrometry. Environ Sci Technol. 2010; 44(10):3690-7. DOI: 10.1021/es903409k. View

16.

Nizkorodov S, Laskin J, Laskin A . Molecular chemistry of organic aerosols through the application of high resolution mass spectrometry. Phys Chem Chem Phys. 2011; 13(9):3612-29. DOI: 10.1039/c0cp02032j. View

17.

Noziere B, Dziedzic P, Cordova A . Inorganic ammonium salts and carbonate salts are efficient catalysts for aldol condensation in atmospheric aerosols. Phys Chem Chem Phys. 2010; 12(15):3864-72. DOI: 10.1039/b924443c. View

18.

De Haan D, Corrigan A, Smith K, Stroik D, Turley J, Lee F . Secondary organic aerosol-forming reactions of glyoxal with amino acids. Environ Sci Technol. 2009; 43(8):2818-24. DOI: 10.1021/es803534f. View

19.

McNeill V . Aqueous organic chemistry in the atmosphere: sources and chemical processing of organic aerosols. Environ Sci Technol. 2015; 49(3):1237-44. DOI: 10.1021/es5043707. View

20.

Laskin J, Laskin A, Roach P, Slysz G, Anderson G, Nizkorodov S . High-resolution desorption electrospray ionization mass spectrometry for chemical characterization of organic aerosols. Anal Chem. 2010; 82(5):2048-58. DOI: 10.1021/ac902801f. View