Dataset Information

Constraining Emissions of Volatile Organic Compounds Over the Indian Subcontinent Using Space-Based Formaldehyde Measurements.

ABSTRACT: India is an air pollution mortality hot spot, but regional emissions are poorly understood. We present a high-resolution nested chemical transport model (GEOS-Chem) simulation for the Indian subcontinent and use it to interpret formaldehyde (HCHO) observations from two satellite sensors (OMI and GOME-2A) in terms of constraints on regional volatile organic compound (VOC) emissions. We find modeled biogenic VOC emissions to be overestimated by ~30-60% for most locations and seasons, and derive a best estimate biogenic flux of 16 Tg C/year subcontinent-wide for year 2009. Terrestrial vegetation provides approximately half the total VOC flux in our base-case inversions (full uncertainty range: 44-65%). This differs from prior understanding, in which biogenic emissions represent >70% of the total. Our derived anthropogenic VOC emissions increase slightly (13-16% in the base case, for a subcontinent total of 15 Tg C/year in 2009) over RETRO year 2000 values, with some larger regional discrepancies. The optimized anthropogenic emissions agree well with the more recent CEDS inventory, both subcontinent-wide (within 2%) and regionally. An exception is the Indo-Gangetic Plain, where we find an underestimate for both RETRO and CEDS. Anthropogenic emissions thus constitute 37-50% of the annual regional VOC source in our base-case inversions and exceed biogenic emissions over the Indo-Gangetic Plain, West India, and South India, and over the entire subcontinent during winter and post-monsoon. Fires are a minor fraction (<7%) of the total regional VOC source in the prior and optimized model. However, evidence suggests that VOC emissions in the fire inventory used here (GFEDv4) are too low over the Indian subcontinent.

SUBMITTER: Chaliyakunnel S

PROVIDER: S-EPMC7894393 | biostudies-literature | 2019 Oct

REPOSITORIES: biostudies-literature

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Constraining Emissions of Volatile Organic Compounds Over the Indian Subcontinent Using Space-Based Formaldehyde Measurements.

Chaliyakunnel Sreelekha S Millet Dylan B DB Chen Xin X

Journal of geophysical research. Atmospheres : JGR 20190830 19

India is an air pollution mortality hot spot, but regional emissions are poorly understood. We present a high-resolution nested chemical transport model (GEOS-Chem) simulation for the Indian subcontinent and use it to interpret formaldehyde (HCHO) observations from two satellite sensors (OMI and GOME-2A) in terms of constraints on regional volatile organic compound (VOC) emissions. We find modeled biogenic VOC emissions to be overestimated by ~30-60% for most locations and seasons, and derive a ...[more]

PMID: 33614368

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Project description:The characterization of vehicle exhaust emissions of volatile organic compounds (VOCs) is essential to estimate their impact on the formation of secondary organic aerosol (SOA) and, more generally, air quality. This paper revises and updates non-methane volatile organic compounds (NMVOCs) tailpipe emissions of three Euro 5 vehicles during Artemis cold urban (CU) and motorway (MW) cycles. Positive matrix factorization (PMF) analysis is carried out for the first time on proton transfer reaction time-of-flight mass spectrometer (PTR-ToF-MS) datasets of vehicular emission. Statistical analysis helped to associate the emitted VOCs to specific driving conditions, such as the start of the vehicles, the activation of the catalysts, or to specific engine combustion regimes. Merged PTR-ToF-MS and automated thermal desorption gas chromatography mass spectrometer (ATD-GC-MS) datasets provided an exhaustive description of the NMVOC emission factors (EFs) of the vehicles, thus helping to identify and quantify up to 147 individual compounds. In general, emissions during the CU cycle exceed those during the MW cycle. The gasoline direct injection (GDI) vehicle exhibits the highest EF during both CU and MW cycles (252 and 15 mg/km), followed by the port-fuel injection (PFI) vehicle (24 and 0.4 mg/km), and finally the diesel vehicle (15 and 3 mg/km). For all vehicles, emissions are dominated by unburnt fuel and incomplete combustion products. Diesel emissions are mostly represented by oxygenated compounds (65%) and aliphatic hydrocarbons (23%) up to C22, while GDI and PFI exhaust emissions are composed of monoaromatics (68%) and alkanes (15%). Intermediate volatility organic compounds (IVOCs) range from 2.7 to 13% of the emissions, comprising essentially linear alkanes for the diesel vehicle, while naphthalene accounts up to 42% of the IVOC fraction for the gasoline vehicles. This work demonstrates that PMF analysis of PTR-ToF-MS datasets and GC-MS analysis of vehicular emissions provide a revised and deep characterization of vehicular emissions to enrich current emission inventories.

Project description:Human occupants themselves constitute an important source of volatile organic compounds (VOCs) in indoor environments through breath and dermal emissions. In order to quantify VOC emissions from occupants under real-world settings, previous indoor observational studies often determined emission factors (i.e., average emission rates per person). However, the values obtained across these studies exhibited large variability, and the causes of this variability still need to be understood. Herein we report 10-day real-time VOC measurements in a university student office, using a proton transfer reaction-quadrupole interface-time-of-flight mass spectrometer. A method was developed to identify VOCs of primary human origin and to quantify the corresponding emission factors, accounting for the dynamically changing occupancy level and ventilation rate in the assessed office. We found that the emission factors of many dermally emitted VOCs strongly increased as the ozone concentration increased from <3 to 10-15 ppb. These VOCs include geranyl acetone, 6-methyl-5-hepten-2-one (6-MHO), and C10-C12 saturated aldehydes, which align with characteristic first-generation ozonolysis products of skin oil. The strongest increase occurred for 6-MHO, from 113 to 337 μg/h/p. In comparison, acetone and isoprene, which are primarily emitted from human breath, varied little with the ozone level. In light of this finding, we conducted an integrated analysis of emission factors reported in the literature for two frequently reported species, namely, 6-MHO and decanal. Ozone concentration alone can explain 94-97% of the variation in their emission factors across previous studies, and the best-estimated ozone dependence obtained using the literature data is consistent with those obtained in the current study. These results suggest that the ozone concentration is a key factor regulating emission factors of many dermally emitted VOCs in real indoor environments, which has to be considered when reporting or using the emission factors.

Dataset Information

Constraining Emissions of Volatile Organic Compounds Over the Indian Subcontinent Using Space-Based Formaldehyde Measurements.

Publications

Constraining Emissions of Volatile Organic Compounds Over the Indian Subcontinent Using Space-Based Formaldehyde Measurements.

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