Contribution Of Wood Combustion Research Articles

Organic aerosol source apportionment in Zurich using an extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF-MS) – Part 2: Biomass burning influences in winter

Abstract. Real-time, in situ molecular composition measurements of the organic fraction of fine particulate matter (PM2.5) remain challenging, hindering a full understanding of the climate impacts and health effects of PM2.5. In particular, the thermal decomposition and ionization-induced fragmentation affecting current techniques has limited a detailed investigation of secondary organic aerosol (SOA), which typically dominates OA. Here we deploy a novel extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF-MS) during winter 2017 in downtown Zurich, Switzerland, which overcomes these limitations, together with an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS) and supporting instrumentation. Positive matrix factorization (PMF) implemented within the Multilinear Engine (ME-2) program was applied to the EESI-TOF-MS data to quantify the primary and secondary contributions to OA. An 11-factor solution was selected as the best representation of the data, including five primary and six secondary factors. Primary factors showed influence from cooking, cigarette smoke, biomass burning (two factors) and a special local unknown event occurred only during two nights. Secondary factors were affected by biomass burning (three factors, distinguished by temperature and/or wind direction), organonitrates, monoterpene oxidation, and undetermined regional processing, in particular the contributions of wood combustion. While the AMS attributed slightly over half the OA mass to SOA but did not identify its source, the EESI-TOF-MS showed that most (>70 %) of the SOA was derived from biomass burning. Together with significant contributions from less aged biomass burning factors identified by both AMS and EESI-TOF-MS, this firmly establishes biomass burning as the single most important contributor to OA mass at this site during winter. High correlation was obtained between EESI-TOF-MS and AMS PMF factors where specific analogues existed, as well as between total signal and POA–SOA apportionment. This suggests the EESI-TOF-MS apportionment in the current study can be approximately taken at face value, despite ion-by-ion differences in relative sensitivity. The apportionment of specific ions measured by the EESI-TOF-MS (e.g., levoglucosan, nitrocatechol, and selected organic acids) and utilization of a cluster analysis-based approach to identify key marker ions for the EESI-TOF-MS factors are investigated. The interpretability of the EESI-TOF-MS results and improved source separation relative to the AMS within this pilot campaign validate the EESI-TOF-MS as a promising approach to source apportionment and atmospheric composition research.

Comparative source apportionment of PM10 in Switzerland for 2008/2009 and 1998/1999 by Positive Matrix Factorisation

PM10 speciation data from various sites in Switzerland for two time periods (January 1998–March 1999 and August 2008–July 2009) have been analysed for major sources by receptor modelling using Positive Matrix Factorisation (PMF). For the 2008/2009 period, it was found that secondary aerosols (sulphate- and nitrate-rich secondary aerosols, SSA and NSA) are the most abundant components of PM10 at sites north of the Alps. Road traffic and wood combustion were found to be the largest sources of PM10 at these sites. Except at the urban roadside site where road traffic is dominating (40% of PM10 -- including road salt), the annual average contribution of these two sources is of similar importance (17% and 14% of PM10, respectively). At a rural site south of the Alps wood combustion and road traffic contributions to PM10 were higher (31% and 24%, respectively), and the fraction of secondary aerosols lower (29%) than at similar site types north of the Alps.Comparison of PMF analyses for the two time periods (1998/1999 and 2008/2009) revealed decreasing average contributions of road traffic and SSA to PM10 at all sites. This indicates that the measures that were implemented in Switzerland and in neighbouring countries to reduce emissions of sulphur dioxide and PM10 from road traffic were successful. On the other hand, contributions of wood combustion did not change during this ten year period, and the contribution of nitrate-rich secondary aerosols has even increased. It is shown that PMF can be a helpful tool for the assessment of long-term changes of source contributions to ambient particulate matter.