Chemical Composition, Sources and Formation Mechanisms of Particulate Brown Carbon in the Atmosphere

doi:10.7536/PC190917

Particulate brown carbon(BrC) has strong wavelength dependence with absorption increasing sharply from visible to UV ranges and has attracted much attention due to its significant climate effects. The composition, sources, evolution and optical properties of BrC remain highly uncertain, which contributes significantly to the uncertainty in estimating aerosol radiation forcing by climate models. The chemical compositions, sources and formation pathways of particulate BrC in the atmosphere are summarized in this review, which focuses on the relationship between molecular-level compositions, secondary formation mechanisms and light absorption properties. Particulate BrC are classfied into several major compound categories, including methanol soluble organic carbon(MSOC), water soluble fractions WSOC(Water Soluble Organic Carbon) and HULIS-C(Carbon Component of HUmic-like Substances). Nitroaromatic compounds(NACs) and N-heterocyclic compounds are major BrC chromophores. The sources of BrC include primary emissions from inefficient combustion, especially biomass burning, and secondary formation via the oxidation of volatile organic compounds(VOCs) in gas and particle phases. Secondary formation pathways include oxidation of aromatics and reactions between carbonyls and ammonia/amines. Oxidation of anthropogenic aromatic hydrocarbons in the presence of NO_x produces BrC dominated by nitrogen-containing organic compounds(e.g. NACs). Reactions between carbonyls and ammonia/amines generate BrC dominated by N-heterocyclic compounds and oligomers. Precursors and reaction conditions are important factors influencing the compositions and light absorption of secondary BrC. The chromophores would go through decomposition and BrC light absorption would change rapidly during transport in the atmosphere, which is usually named photobleaching. Molecular-level identification of BrC chromophores and further understanding on the secondary formation mechanisms and atmospheric evolution of BrC are required in future studies.

Contents

1 Introduction

2 Measurements of BrC

3 Chemical composition of BrC

3.1 Major compound categories

3.2 Molecular compositions

4 Sources of BrC

4.1 Source apportionment

4.2 Biomass burning emissions

5 Secondary formation pathways of BrC

5.1 BrC from oxidation of anthropogenic aromatic precursors

5.2 BrC from reactions between carbonyls and ammonia/amines

5.3 Atmospheric aging of BrC

6 Conclusion and outlook

Key words: brown carbon(BrC), secondary formation mechanisms, source, chemical composition, nitroaromatic compounds(NACs), N-heterocyclic compounds

Fig. 1 Classification and molecular composition of carbonaceous aerosol components[4]

Fig. 2 The observed concentrations of carbon component of HUmic-LIke Substances(HULIS-C), water soluble organic carbon(WSOC) and their ratios in different atmospheric environments[46, 48~76].The concentrations in Asia correspond to the right axis and others correspond to the left axis. Gray, green and blue backgrounds demote the urban site, rural/suburban site and clean site, respectively. The clean site include mountain/highland site, marine and Arctic sites. The markers “sp”, “su”, “a”, “w” and “y” in parentheses represent the studies conducted in spring, summer, autumn, winter or yearly round, respectively. The site names marked by “*” are reported in this study

Table 1 List of nitrogen-containing organic compounds contributing to the light absorption by particulate BrC

Formula	Sources			ref	Formula	Sources		ref
Formula	Oxidation of aromatic VOCs	Biomass burning	MG+AS ^a	ref	Formula	Biomass burning	MG+AS ^a	ref
C₅H₄N₂O₅	√			21	C₁₃H₁₃NO₃	√		84
C₆H₃N₃O₇	√			21	C₁₃H₁₃NO₄	√		86
C₆H₄N₂O₅	√			21	C₁₅H₂₃N₃O₂	√		91
C₆H₄N₂O₆	√			21, 92	C₁₆H₉NO₃	√		84
C₆H₅NO₂	√			21	C₁₇H₁₁N	√		86
C₆H₅NO₃	√	√		17, 21, 85, 87, 90, 92	C₁₈H₂₇NO₅	√		84
C₆H₅NO₄	√	√		17, 84, 85, 87, 90, 92	C₂₁H₁₁N	√		84, 86
C₆H₅NO₅	√	√		84~86, 92	C₂₁H₁₃N	√		84
C₆H₆N₂O₆	√			21	C₂₂H₃₄N₂O₆	√		84
C₇H₄N₂O₆	√			21	C₂₃H₁₃N	√		84
C₇H₄N₂O₇	√			21	C₂₃H₃₁NO₄	√		84
C₇H₅NO₆	√			21	C₂₇H₃₉NO₂	√		84
C₇H₆N₂O₆	√			21, 92	C₄₈H₆₆N₄O₄	√		84
C₇H₇NO₂	√			21	C₆H₇NO₂		√	88
C₇H₇NO₃	√	√		17, 21, 85, 87, 90~92	C₆H₈N₂		√	88
C₇H₇NO₄	√	√		17, 21, 84~87, 90~92	C₆H₈N₂O		√	88
C₇H₇NO₅	√	√		21, 84, 85, 87, 92	C₆H₉NO₃		√	88
C₇H₈N₂O₇	√			21	C₇H₁₀N₂O		√	88
C₇H₉NO₅	√			21	C₈H₁₀N₂O		√	88
C₈H₇NO₄	√	√		17, 84, 86, 92	C₈H₁₁NO		√	88
C₈H₈N₂O₅	√			21	C₈H₁₁NO₃		√	88
C₈H₉NO₄	√	√		85~87, 92	C₈H₁₂N₂O		√	88
C₈H₉NO₅	√	√		17, 84~87, 92	C₈H₇NO₂		√	88
C₈H₁₃NO₈	√			21	C₉H₁₁N₃		√	88
C₉H₉NO₄	√	√		17, 85, 87, 92	C₉H₁₁N₃O		√	88
C₁₀H₇NO₄	√			92	C₉H₁₁NO₃		√	88
C₅H₄N₂O₃		√		85	C₉H₁₂N₂O		√	88
C₅H₅NO₄		√		85	C₉H₉NO₃		√	88
C₆H₄N₂O₅		√		85, 90	C₁₀H₁₁NO₂		√	88
C₆H₆N₂O₃		√		85	C₁₀H₁₃N₃O		√	88
C₇H₅NO₅		√		85, 91, 92	C₁₀H₁₄N₂O₄		√	88
C₇H₆N₂O₅		√		85	C₁₁H₁₄N₂O₃		√	88
C₈H₅NO₄		√		85	C₁₁H₁₄N₂O₄		√	88
C₈H₇NO₃		√		84, 87	C₁₁H₁₅NO₆		√	88
C₈H₈N₂O₅		√		85	C₁₁H₁₇N₃O₃		√	88
C₈H₉NO₃		√		85, 91	C₁₂H₁₄N₂O₃		√	88
C₉H₁₁NO₄		√	√	85, 86, 88	C₁₂H₁₄N₂O₄		√	88
C₉H₇NO₃		√		84	C₁₂H₁₅N₃O₃		√	88
C₉H₇NO₄		√		84, 85	C₁₂H₁₆N₂O₄		√	88
C₉H₉NO₅		√		85	C₁₂H₁₆N₂O₅		√	88
C₁₀H₁₀N₂O₇		√		85	C₁₃H₁₆N₂O₂		√	88
C₁₀H₁₁NO₄		√		85	C₁₃H₁₇N₃O₃		√	88
C₁₀H₁₁NO₅		√		85, 86	C₁₃H₁₈N₂O₆		√	88
C₁₀H₁₃NO₄		√		86	C₁₄H₁₆N₂O₂		√	88
C₁₀H₇NO₃		√		84~86, 92	C₁₄H₁₇N₃O₃		√	88
C₁₀H₇NO₅		√		85	C₁₅H₁₇N₃O₃		√	88
C₁₀H₈N₂O₃		√		85	C₁₅H₁₉NO₆		√	88
C₁₀H₉NO₅		√		85	C₁₅H₂₁N₃O₆		√	88
C₁₁H₁₁NO₄		√		85	C₁₅H₂₁NO₇		√	88
C₁₁H₁₃NO₄		√		86	C₁₇H₁₉NO₅		√	88
C₁₁H₁₃NO₅		√		86	C₁₇H₂₀N₂O₆		√	88
C₁₁H₉NO₃		√		84	C₁₇H₂₀N₂O₇		√	88
C₁₂H₁₁NO₃		√		84	C₁₈H₂₃N₃O₅		√	88

Table 1 List of nitrogen-containing organic compounds contributing to the light absorption by particulate BrC

Formula	Sources			ref	Formula	Sources		ref
Formula	Oxidation of aromatic VOCs	Biomass burning	MG+AS ^a	ref	Formula	Biomass burning	MG+AS ^a	ref
C₅H₄N₂O₅	√			21	C₁₃H₁₃NO₃	√		84
C₆H₃N₃O₇	√			21	C₁₃H₁₃NO₄	√		86
C₆H₄N₂O₅	√			21	C₁₅H₂₃N₃O₂	√		91
C₆H₄N₂O₆	√			21, 92	C₁₆H₉NO₃	√		84
C₆H₅NO₂	√			21	C₁₇H₁₁N	√		86
C₆H₅NO₃	√	√		17, 21, 85, 87, 90, 92	C₁₈H₂₇NO₅	√		84
C₆H₅NO₄	√	√		17, 84, 85, 87, 90, 92	C₂₁H₁₁N	√		84, 86
C₆H₅NO₅	√	√		84~86, 92	C₂₁H₁₃N	√		84
C₆H₆N₂O₆	√			21	C₂₂H₃₄N₂O₆	√		84
C₇H₄N₂O₆	√			21	C₂₃H₁₃N	√		84
C₇H₄N₂O₇	√			21	C₂₃H₃₁NO₄	√		84
C₇H₅NO₆	√			21	C₂₇H₃₉NO₂	√		84
C₇H₆N₂O₆	√			21, 92	C₄₈H₆₆N₄O₄	√		84
C₇H₇NO₂	√			21	C₆H₇NO₂		√	88
C₇H₇NO₃	√	√		17, 21, 85, 87, 90~92	C₆H₈N₂		√	88
C₇H₇NO₄	√	√		17, 21, 84~87, 90~92	C₆H₈N₂O		√	88
C₇H₇NO₅	√	√		21, 84, 85, 87, 92	C₆H₉NO₃		√	88
C₇H₈N₂O₇	√			21	C₇H₁₀N₂O		√	88
C₇H₉NO₅	√			21	C₈H₁₀N₂O		√	88
C₈H₇NO₄	√	√		17, 84, 86, 92	C₈H₁₁NO		√	88
C₈H₈N₂O₅	√			21	C₈H₁₁NO₃		√	88
C₈H₉NO₄	√	√		85~87, 92	C₈H₁₂N₂O		√	88
C₈H₉NO₅	√	√		17, 84~87, 92	C₈H₇NO₂		√	88
C₈H₁₃NO₈	√			21	C₉H₁₁N₃		√	88
C₉H₉NO₄	√	√		17, 85, 87, 92	C₉H₁₁N₃O		√	88
C₁₀H₇NO₄	√			92	C₉H₁₁NO₃		√	88
C₅H₄N₂O₃		√		85	C₉H₁₂N₂O		√	88
C₅H₅NO₄		√		85	C₉H₉NO₃		√	88
C₆H₄N₂O₅		√		85, 90	C₁₀H₁₁NO₂		√	88
C₆H₆N₂O₃		√		85	C₁₀H₁₃N₃O		√	88
C₇H₅NO₅		√		85, 91, 92	C₁₀H₁₄N₂O₄		√	88
C₇H₆N₂O₅		√		85	C₁₁H₁₄N₂O₃		√	88
C₈H₅NO₄		√		85	C₁₁H₁₄N₂O₄		√	88
C₈H₇NO₃		√		84, 87	C₁₁H₁₅NO₆		√	88
C₈H₈N₂O₅		√		85	C₁₁H₁₇N₃O₃		√	88
C₈H₉NO₃		√		85, 91	C₁₂H₁₄N₂O₃		√	88
C₉H₁₁NO₄		√	√	85, 86, 88	C₁₂H₁₄N₂O₄		√	88
C₉H₇NO₃		√		84	C₁₂H₁₅N₃O₃		√	88
C₉H₇NO₄		√		84, 85	C₁₂H₁₆N₂O₄		√	88
C₉H₉NO₅		√		85	C₁₂H₁₆N₂O₅		√	88
C₁₀H₁₀N₂O₇		√		85	C₁₃H₁₆N₂O₂		√	88
C₁₀H₁₁NO₄		√		85	C₁₃H₁₇N₃O₃		√	88
C₁₀H₁₁NO₅		√		85, 86	C₁₃H₁₈N₂O₆		√	88
C₁₀H₁₃NO₄		√		86	C₁₄H₁₆N₂O₂		√	88
C₁₀H₇NO₃		√		84~86, 92	C₁₄H₁₇N₃O₃		√	88
C₁₀H₇NO₅		√		85	C₁₅H₁₇N₃O₃		√	88
C₁₀H₈N₂O₃		√		85	C₁₅H₁₉NO₆		√	88
C₁₀H₉NO₅		√		85	C₁₅H₂₁N₃O₆		√	88
C₁₁H₁₁NO₄		√		85	C₁₅H₂₁NO₇		√	88
C₁₁H₁₃NO₄		√		86	C₁₇H₁₉NO₅		√	88
C₁₁H₁₃NO₅		√		86	C₁₇H₂₀N₂O₆		√	88
C₁₁H₉NO₃		√		84	C₁₇H₂₀N₂O₇		√	88
C₁₂H₁₁NO₃		√		84	C₁₈H₂₃N₃O₅		√	88

Fig. 3 Secondary formation pathways of nitroaromatic compounds in gas and particle phases[24, 25, 111~114]

Fig. 4 Proposed reaction pathways for the formation of imidazole and other N-heterocyclic compounds in the glyoxal/ammonium sulfate system[128,129,130]

Fig. 5 The research framework of brown carbon

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Chemical Composition, Sources and Formation Mechanisms of Particulate Brown Carbon in the Atmosphere

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Chemical Composition, Sources and Formation Mechanisms of Particulate Brown Carbon in the Atmosphere