University of Groningen Characterization and source apportionment of carbonaceous aerosols in China Ni, Haiyan

University of Groningen

Characterization and source apportionment of carbonaceous aerosols in China

Ni, Haiyan

DOI:

10.33612/diss.79450942

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Publication date: 2019

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Ni, H. (2019). Characterization and source apportionment of carbonaceous aerosols in China. University of Groningen. https://doi.org/10.33612/diss.79450942

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Characterization and

Source Apportionment of

Carbonaceous Aerosols in

China

Characterization and Source Apportionment of Carbonaceous Aerosols in China Haiyan Ni PhD thesis, 2019 University of Groningen The Netherlands ISBN: 978-94-034-1585-7 ISBN: 978-94-034-1584-0 (Ebook) Printed by Proefschrift Maken, Utrecht Cover designed by H. Ni and TM DESIGN

The research presented in this thesis was performed at the Centre for Isotope Research (CIO), which is part of the Energy and Sustainability Research Institute Groningen (ESRIG) of the University of Groningen, the Netherlands.

Characterization and

Source Apportionment of

Carbonaceous Aerosols in

China

PhD thesis

to obtain the degree of PhD at the

University of Groningen

on the authority of the

Rector Magnificus prof. E. Sterken

and in accordance with

the decision by the College of Deans.

This thesis will be defended in public on

Monday 15 April 2019 at 12.45 hours

by

Haiyan Ni

born on 30 June 1988

in Tianjin, China

Supervisor

Prof. H.A.J. Meijer

Co-supervisor

Assessment Committee

Contents

1 Introduction ... 9

1.1 Aerosol ... 10

1.2 Carbonaceous aerosols ... 12

1.3 Light absorption of brown carbon ... 14

1.4 Volatility and aging of organic aerosols (OA) ... 17

1.5 Source apportionment of carbonaceous aerosols ... 19

1.6 Ambient PM2.5 pollution in China ... 26

1.7 Motivation and thesis outline ... 29

References ... 31

2 Source apportionment of carbonaceous aerosols in Xi’an, China: insights from a full year of measurements of radiocarbon and the stable isotope 13_{C ... 37}

2.1. Introduction ... 38

2.2 Methods ... 43

2.2.1 Sampling ... 43

2.2.2 Organic carbon (OC), elemental carbon (EC), and source markers’ measurement ... 44

2.2.3 Stable carbon isotopic composition of OC and EC ... 44

2.2.4 Radiocarbon (14_{C) measurement of OC and EC ... 45}

2.2.5 Source apportionment methodology using 14_{C ... 46}

2.2.6 Source apportionment of EC using Bayesian statistics ... 47

2.3. Results ... 48

2.3.1 Temporal variation of OC and EC mass concentrations ... 48

2.3.2 Temporal variation of fossil and non-fossil fractions of OC and EC49 2.3.3 13_{C signature of OC and EC ... 51}

2.4 Discussion ... 53

2.4.2 Correlations between F14_C

(EC) and biomass burning markers ... 54

2.4.3 δ13_C/F14_{C-based statistical source apportionment of EC... 55}

2.4.4 Estimating mass concentrations and sources of primary OC ... 60

2.4.5 Differences between observed and estimated primary OC concentrations and sources ... 63

2.4.6 Changes in emission sources in Xi’an, China (2008/2009 vs. 2012/2013) ... 65

2.5 Conclusions ... 67

Acknowledgments ... 69

References ... 70

S2. Supplement ... 78

3 High contributions of fossil sources to more volatile organic carbon ... 103

3.1 Introduction ... 104

3.2 Methods ... 107

3.2.1 Sampling ... 107

3.2.2 Determination of carbon fractions by thermal-optical analysis ... 108

3.2.3 Radiocarbon (14_{C) measurements of mvOC, OC and EC ... 108}

3.2.4 Estimation of source contributions to different carbon fractions ... 111

3.3 Results ... 113

3.3.1 Method evaluation and quality control for mvOC extraction ... 113

3.3.2 mvOC, OC and EC concentrations ... 116

3.3.3 Non-fossil and fossil fractions of different carbon fractions ... 118

3.4 Discussion ... 125

3.5 Conclusions ... 128

Acknowledgments ... 130

Reference ... 131

S3. Supplement ... 138

4 Light-absorbing organic carbon in aerosol extracts from primary and aged coal combustion emissions ... 155

4.2 Methods ... 158

4.2.1 Experimental setup ... 158

4.2.2 Off-line UV-Vis measurements and light absorption calculation .. 159

4.3 Results and discussion ... 161

4.3.1 Light absorption spectra ... 161

4.3.2 Bulk mass absorption coefficient (bulk MAC) of the methanol extracts ... 163

4.3.3 Methanol-extracted bulk MAC365nm ... 164

4.4 Comparison with previous studies ... 170

4.5 Conclusion ... 172

Acknowledgment ... 173

Reference ... 174

S4. Supplement ... 182

5 Conclusion and Outlook ... 191

5.1 Sources of different carbon fractions of carbonaceous aerosols ... 192

5.2 Light absorption of primary and aged coal combustion emissions ... 202

References ... 204

Summary 207

Samenvatting 211

Acknowledgements 215