RESUMEN
The use of hydraulic fracturing for production of petroleum and natural gas has increased dramatically in the past decade, but the environmental impacts of this technology remain unclear. Experiments were conducted to quantify airborne emissions from 12 samples of hydraulic fracturing flowback wastewater collected in the Permian Basin, as well as the photochemical processing of these emissions leading to the formation of particulate matter (PM). The concentration of total volatile carbon (hydrocarbons evaporating at room temperature) averaged 29 mg of carbon per liter. After photochemical oxidation under high NO x conditions, the amount of organic PM formed per milliliter of wastewater evaporated averaged 24 µg; the amount of ammonium nitrate formed averaged 262 µg. Based on the mean PM formation observed in these experiments, the estimated formation of PM from evaporated flowback wastewater in the state of Texas is in the range of estimated PM emissions from diesel engines used in oil rigs. Evaporation of flowback wastewater, a hitherto unrecognized source of secondary pollutants, could significantly contribute to ambient PM concentrations.
Asunto(s)
Fracking Hidráulico , Gas Natural , Material Particulado , Texas , Aguas ResidualesRESUMEN
The House Observations of Microbial and Environmental Chemistry (HOMEChem) study is a collaborative field investigation designed to probe how everyday activities influence the emissions, chemical transformations and removal of trace gases and particles in indoor air. Sequential and layered experiments in a research house included cooking, cleaning, variable occupancy, and window-opening. This paper describes the overall design of HOMEChem and presents preliminary case studies investigating the concentrations of reactive trace gases, aerosol particles, and surface films. Cooking was a large source of VOCs, CO2, NOx, and particles. By number, cooking particles were predominantly in the ultrafine mode. Organic aerosol dominated the submicron mass, and, while variable between meals and throughout the cooking process, was dominated by components of hydrocarbon character and low oxygen content, similar to cooking oil. Air exchange in the house ensured that cooking particles were present for only short periods. During unoccupied background intervals, particle concentrations were lower indoors than outdoors. The cooling coils of the house ventilation system induced cyclic changes in water soluble gases. Even during unoccupied periods, concentrations of many organic trace gases were higher indoors than outdoors, consistent with housing materials being potential sources of these compounds to the outdoor environment. Organic material accumulated on indoor surfaces, and exhibited chemical signatures similar to indoor organic aerosol.
Asunto(s)
Microbiología del Aire/normas , Contaminantes Atmosféricos/análisis , Contaminación del Aire Interior/análisis , Monitoreo del Ambiente/métodos , Vivienda/normas , Material Particulado/análisis , Aerosoles , Aire Acondicionado , Filtros de Aire , Culinaria , Gases , Humanos , Tamaño de la PartículaRESUMEN
The sources of submicrometer particulate matter (PM1) remain poorly characterized in the industrialized city of Houston, TX. A mobile sampling approach was used to characterize PM1 composition and concentration across Houston based on high-time-resolution measurements of nonrefractory PM1 and trace gases during the DISCOVER-AQ Texas 2013 campaign. Two pollution zones with marked differences in PM1 levels, character, and dynamics were established based on cluster analysis of organic aerosol mass loadings sampled at 16 sites. The highest PM1 mass concentrations (average 11.6 ± 5.7 µg/m3) were observed to the northwest of Houston (zone 1), dominated by secondary organic aerosol (SOA) mass likely driven by nighttime biogenic organonitrate formation. Zone 2, an industrial/urban area south/east of Houston, exhibited lower concentrations of PM1 (average 4.4 ± 3.3 µg/m3), significant organic aerosol (OA) aging, and evidence of primary sulfate emissions. Diurnal patterns and backward-trajectory analyses enable the classification of airmass clusters characterized by distinct PM sources: biogenic SOA, photochemical aged SOA, and primary sulfate emissions from the Houston Ship Channel. Principal component analysis (PCA) indicates that secondary biogenic organonitrates primarily related with monoterpenes are predominant in zone 1 (accounting for 34% of the variability in the data set). The relevance of photochemical processes and industrial and traffic emission sources in zone 2 also is highlighted by PCA, which identifies three factors related with these processes/sources (~50% of the aerosol/trace gas concentration variability). PCA reveals a relatively minor contribution of isoprene to SOA formation in zone 1 and the absence of isoprene-derived aerosol in zone 2. The relevance of industrial amine emissions and the likely contribution of chloride-displaced sea salt aerosol to the observed variability in pollution levels in zone 2 also are captured by PCA. IMPLICATIONS: This article describes an urban-scale mobile study to characterize spatial variations in submicrometer particulate matter (PM1) in greater Houston. The data set indicates substantial spatial variations in PM1 sources/chemistry and elucidates the importance of photochemistry and nighttime oxidant chemistry in producing secondary PM1. These results emphasize the potential benefits of effective control strategies throughout the region, not only to reduce primary emissions of PM1 from automobiles and industry but also to reduce the emissions of important secondary PM1 precursors, including sulfur oxides, nitrogen oxides, ammonia, and volatile organic compounds. Such efforts also could aid in efforts to reduce mixing ratios of ozone.