Reactivity of aminophenols in forming nitrogen-containing brown carbon from iron-catalyzed reactions

Hind A. Al-Abadleh; Fatemeh Motaghedi; Wisam Mohammed; Md Sohel Rana; Kotiba A. Malek; Dewansh Rastogi; Akua A. Asa-Awuku; Marcelo I. Guzman

doi:10.1038/s42004-022-00732-1

Reactivity of aminophenols in forming nitrogen-containing brown carbon from iron-catalyzed reactions

Hind A. Al-Abadleh
, Fatemeh Motaghedi
, Wisam Mohammed
, Md Sohel Rana
, Kotiba A. Malek
, Dewansh Rastogi
, Akua A. Asa-Awuku
, Marcelo I. Guzman

Producción científica: Article › revisión exhaustiva

17 Citas (Scopus)

Resumen

Nitrogen-containing organic carbon (NOC) in atmospheric particles is an important class of brown carbon (BrC). Redox active NOC like aminophenols received little attention in their ability to form BrC. Here we show that iron can catalyze dark oxidative oligomerization of o- and p-aminophenols under simulated aerosol and cloud conditions (pH 1–7, and ionic strength 0.01–1 M). Homogeneous aqueous phase reactions were conducted using soluble Fe(III), where particle growth/agglomeration were monitored using dynamic light scattering. Mass yield experiments of insoluble soot-like dark brown to black particles were as high as 40%. Hygroscopicity growth factors (κ) of these insoluble products under sub- and super-saturated conditions ranged from 0.4–0.6, higher than that of levoglucosan, a prominent proxy for biomass burning organic aerosol (BBOA). Soluble products analyzed using chromatography and mass spectrometry revealed the formation of ring coupling products of o- and p-aminophenols and their primary oxidation products. Heterogeneous reactions of aminophenol were also conducted using Arizona Test Dust (AZTD) under simulated aging conditions, and showed clear changes to optical properties, morphology, mixing state, and chemical composition. These results highlight the important role of iron redox chemistry in BrC formation under atmospherically relevant conditions.

Idioma original	English
Número de artículo	112
Publicación	Communications Chemistry
Volumen	5
N.º	1
DOI	https://doi.org/10.1038/s42004-022-00732-1
Estado	Published - dic 2022

Nota bibliográfica

Funding Information:
The authors acknowledge funding from the Natural Science and Engineering Council of Canada (NSERC) and to the U.S.A. National Science Foundation under award 1903744 to M.I.G. For technical assistance, the authors would like to thank Dr. Kitaev at Laurier for DLS, Drs. Smith and Goodfellow from the MS facility at the University of Waterloo for MALDI-TOF-MS, Dr. Castel from the Department of Chemical Engineering at the University of Waterloo for TGA, Dr. Andrei and Victoria Jarvis from the Canadian Centre for Electron Microscopy and MAX Diffraction Facility at McMaster University.

Publisher Copyright:
© 2022, The Author(s).

Financiación

The authors acknowledge funding from the Natural Science and Engineering Council of Canada (NSERC) and to the U.S.A. National Science Foundation under award 1903744 to M.I.G. For technical assistance, the authors would like to thank Dr. Kitaev at Laurier for DLS, Drs. Smith and Goodfellow from the MS facility at the University of Waterloo for MALDI-TOF-MS, Dr. Castel from the Department of Chemical Engineering at the University of Waterloo for TGA, Dr. Andrei and Victoria Jarvis from the Canadian Centre for Electron Microscopy and MAX Diffraction Facility at McMaster University.

Financiadores	Número del financiador
Department of Chemical Engineering, Universiti Teknologi Petronas
University of Waterloo
National Science Foundation Arctic Social Science Program	1903744

ASJC Scopus subject areas

General Chemistry
Environmental Chemistry
Biochemistry
Materials Chemistry

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10.1038/s42004-022-00732-1

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title = "Reactivity of aminophenols in forming nitrogen-containing brown carbon from iron-catalyzed reactions",

abstract = "Nitrogen-containing organic carbon (NOC) in atmospheric particles is an important class of brown carbon (BrC). Redox active NOC like aminophenols received little attention in their ability to form BrC. Here we show that iron can catalyze dark oxidative oligomerization of o- and p-aminophenols under simulated aerosol and cloud conditions (pH 1–7, and ionic strength 0.01–1 M). Homogeneous aqueous phase reactions were conducted using soluble Fe(III), where particle growth/agglomeration were monitored using dynamic light scattering. Mass yield experiments of insoluble soot-like dark brown to black particles were as high as 40\%. Hygroscopicity growth factors (κ) of these insoluble products under sub- and super-saturated conditions ranged from 0.4–0.6, higher than that of levoglucosan, a prominent proxy for biomass burning organic aerosol (BBOA). Soluble products analyzed using chromatography and mass spectrometry revealed the formation of ring coupling products of o- and p-aminophenols and their primary oxidation products. Heterogeneous reactions of aminophenol were also conducted using Arizona Test Dust (AZTD) under simulated aging conditions, and showed clear changes to optical properties, morphology, mixing state, and chemical composition. These results highlight the important role of iron redox chemistry in BrC formation under atmospherically relevant conditions.",

author = "Al-Abadleh, \{Hind A.\} and Fatemeh Motaghedi and Wisam Mohammed and Rana, \{Md Sohel\} and Malek, \{Kotiba A.\} and Dewansh Rastogi and Asa-Awuku, \{Akua A.\} and Guzman, \{Marcelo I.\}",

note = "Funding Information: The authors acknowledge funding from the Natural Science and Engineering Council of Canada (NSERC) and to the U.S.A. National Science Foundation under award 1903744 to M.I.G. For technical assistance, the authors would like to thank Dr. Kitaev at Laurier for DLS, Drs. Smith and Goodfellow from the MS facility at the University of Waterloo for MALDI-TOF-MS, Dr. Castel from the Department of Chemical Engineering at the University of Waterloo for TGA, Dr. Andrei and Victoria Jarvis from the Canadian Centre for Electron Microscopy and MAX Diffraction Facility at McMaster University. Publisher Copyright: {\textcopyright} 2022, The Author(s).",

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AU - Al-Abadleh, Hind A.

AU - Motaghedi, Fatemeh

AU - Mohammed, Wisam

AU - Rana, Md Sohel

AU - Malek, Kotiba A.

AU - Rastogi, Dewansh

AU - Asa-Awuku, Akua A.

AU - Guzman, Marcelo I.

N1 - Funding Information: The authors acknowledge funding from the Natural Science and Engineering Council of Canada (NSERC) and to the U.S.A. National Science Foundation under award 1903744 to M.I.G. For technical assistance, the authors would like to thank Dr. Kitaev at Laurier for DLS, Drs. Smith and Goodfellow from the MS facility at the University of Waterloo for MALDI-TOF-MS, Dr. Castel from the Department of Chemical Engineering at the University of Waterloo for TGA, Dr. Andrei and Victoria Jarvis from the Canadian Centre for Electron Microscopy and MAX Diffraction Facility at McMaster University. Publisher Copyright: © 2022, The Author(s).

PY - 2022/12

Y1 - 2022/12

N2 - Nitrogen-containing organic carbon (NOC) in atmospheric particles is an important class of brown carbon (BrC). Redox active NOC like aminophenols received little attention in their ability to form BrC. Here we show that iron can catalyze dark oxidative oligomerization of o- and p-aminophenols under simulated aerosol and cloud conditions (pH 1–7, and ionic strength 0.01–1 M). Homogeneous aqueous phase reactions were conducted using soluble Fe(III), where particle growth/agglomeration were monitored using dynamic light scattering. Mass yield experiments of insoluble soot-like dark brown to black particles were as high as 40%. Hygroscopicity growth factors (κ) of these insoluble products under sub- and super-saturated conditions ranged from 0.4–0.6, higher than that of levoglucosan, a prominent proxy for biomass burning organic aerosol (BBOA). Soluble products analyzed using chromatography and mass spectrometry revealed the formation of ring coupling products of o- and p-aminophenols and their primary oxidation products. Heterogeneous reactions of aminophenol were also conducted using Arizona Test Dust (AZTD) under simulated aging conditions, and showed clear changes to optical properties, morphology, mixing state, and chemical composition. These results highlight the important role of iron redox chemistry in BrC formation under atmospherically relevant conditions.

AB - Nitrogen-containing organic carbon (NOC) in atmospheric particles is an important class of brown carbon (BrC). Redox active NOC like aminophenols received little attention in their ability to form BrC. Here we show that iron can catalyze dark oxidative oligomerization of o- and p-aminophenols under simulated aerosol and cloud conditions (pH 1–7, and ionic strength 0.01–1 M). Homogeneous aqueous phase reactions were conducted using soluble Fe(III), where particle growth/agglomeration were monitored using dynamic light scattering. Mass yield experiments of insoluble soot-like dark brown to black particles were as high as 40%. Hygroscopicity growth factors (κ) of these insoluble products under sub- and super-saturated conditions ranged from 0.4–0.6, higher than that of levoglucosan, a prominent proxy for biomass burning organic aerosol (BBOA). Soluble products analyzed using chromatography and mass spectrometry revealed the formation of ring coupling products of o- and p-aminophenols and their primary oxidation products. Heterogeneous reactions of aminophenol were also conducted using Arizona Test Dust (AZTD) under simulated aging conditions, and showed clear changes to optical properties, morphology, mixing state, and chemical composition. These results highlight the important role of iron redox chemistry in BrC formation under atmospherically relevant conditions.

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UR - https://www.scopus.com/pages/publications/85138240222#tab=citedBy

U2 - 10.1038/s42004-022-00732-1

DO - 10.1038/s42004-022-00732-1

M3 - Article

AN - SCOPUS:85138240222

VL - 5

JO - Communications Chemistry

JF - Communications Chemistry

IS - 1

M1 - 112

ER -

Reactivity of aminophenols in forming nitrogen-containing brown carbon from iron-catalyzed reactions

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ASJC Scopus subject areas

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