Abstract

Abstract. Black carbon (BC) is known to have major impacts on both human health and climate. The populated megacity represents the most complex anthropogenic BC emissions where the sources and related impacts are very uncertain. This study provides source attribution and characterization of BC in the Beijing urban environment during the joint UK–China APHH (Air Pollution and Human Health) project, in both winter (November–December 2016) and summer (May–June 2017). The size-resolved mixing state of BC-containing particles was characterized by a single-particle soot photometer (SP2) and their mass spectra was measured by a soot particle aerosol mass spectrometer (SP-AMS). The refractory BC (rBC) mass loading was around a factor of 2 higher in winter relative to summer, and more variable coatings were present, likely as a result of additional surface emissions from the residential sector and favourable condensation in the cold season. The characteristics of the BC were relatively independent of air mass direction in summer, whereas in winter air masses from the Northern Plateau were considerably cleaner and contained less-coated and smaller BC, but the BC from the Southern Plateau had the largest core size and coatings. We compare two online source apportionment methods using simultaneous measurements made by the SP2, which measures physical properties of BC, and the chemical approach using the positive matrix factorization (PMF) of mass spectra from the SP-AMS for the first time. A method is proposed to isolate the BC from the transportation sector using a mode of small BC particles (core diameter Dc<0.18 µm and coating thickness ct < 50 nm). This mode of BC highly correlated with NOx concentration in both seasons (∼14 ng m−3 BC ppb−1 NOx) and corresponded with the morning traffic rush hour, contributing about 30 % and 40 % of the total rBC mass (35 % and 55 % in number) in winter and summer respectively. The BC from coal burning or biomass burning was characterized by moderate coatings (ct = 50–200 nm) contributing ∼20 %–25 % of rBC mass. Large uncoated BC particles (Dc>0.18 µm and ct < 50 nm) were more likely to be contributed by coal combustion, as these particles were not present in urban London. This mode was present in Beijing in both winter (∼30 %–40 % rBC mass) and summer (∼40 % rBC mass) but may be dominated by the residential and industrial sector respectively. The contribution of BC thickly coated with secondary species (ct > 200 nm) to the total rBC mass increased with pollution level in winter but was minor in summer. These large BC particles importantly enhanced the absorption efficiency at high pollution levels – in winter when PM1 > 100 µg m−3 or BC > 2 µg m−3, the absorption efficiency of BC increased by 25 %–70 %. The reduction of emissions of these large BC particles and the precursors of the associated secondary coating will be an effective way of mitigating the heating effect of BC in urban environments.

Highlights

  • Black carbon aerosol (BC) has a significant impact on both climate (Bond et al, 2013) and human health (Baumgartner et al, 2014)

  • Each property is discussed in turn and the similarities and differences between the seasons highlighted to clearly identify property changes that can be linked to changes in sources or processes in summer and winter

  • The first half of the winter campaign up to 20 November was periodically influenced by air masses from the Western North China Plain (NCP), and during the second half the synoptic meteorology shifted appreciably and was dominated by northerly or westerly air masses, with the period between 2 and 4 December dominated by air from the Southern Plateau

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Summary

Introduction

Black carbon aerosol (BC) has a significant impact on both climate (Bond et al, 2013) and human health (Baumgartner et al, 2014). The BC sources in Beijing are combinations of residential, industrial and transport sectors (Li et al, 2017), and the fuel use could be rather more complex than two distinct sources on which most techniques are based Both coal burning and diesel fuel could emit fossil fuel BC, which may not be isolated through isotope analysis, and the absorption spectrum of BC from different sources may vary considerably, and to assume a single pattern based on Aethalometer measurements may not be suitable to attribute multiple sources. All the points along a single trajectory are used to determine the fraction of time during the previous day that the air mass spent above each of the classified regions as shown in the bottom panel of Fig. 3a and b This method has been applied previously in the western Africa region to identify the potential source contributions (Liu et al, 2018). The planetary boundary layer height (PBLH) spanning the experimental period was determined using lidar and ceilometer measurements (Kotthaus and Grimmond, 2018)

The physical properties of BC
BC chemical composition
Overview of BC physical properties
The size distribution and mixing state of BC
BC segregation by size-resolved mixing state
Comparison of BC source estimation
Diurnal variation of different types of BC
BC at different pollution levels
Conclusions
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