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The recent regulatory spotlight on continuous monitoring (CM) solutions and the rapid development of CM solutions have demanded the characterization of solution performance through regular, rigorous testing using consensus test protocols. This study is the second known implementation of such a protocol involving single-blind controlled testing of 9 CM solutions. Controlled releases of rates (6-7100 g) CH4/h over durations (0.4-10.2 h) under a wind speed range of (0.7-9.9 m/s) were conducted for 11 weeks. Results showed that 4 solutions achieved method detection limits (DL90s) within the tested emission rate range, with all 4 solutions having both the lowest DL90s (3.9 [3.0, 5.5] kg CH4/h to 6.2 [3.7, 16.7] kg CH4/h) and false positive rates (6.9-13.2%), indicating efforts at balancing low sensitivity with a low false positive rate. These results are likely best-case scenario estimates since the test center represents a near-ideal upstream field natural gas operation condition. Quantification results showed wide individual estimate uncertainties, with emissions underestimation and overestimation by factors up to >14 and 42, respectively. Three solutions had >80% of their estimates within a quantification factor of 3 for controlled releases in the ranges of [0.1-1] kg CH4/h and > 1 kg CH4/h. Relative to the study by Bell et al., current solutions performance, as a group, generally improved, primarily due to solutions from the study by Bell et al. that were retested. This result highlights the importance of regular quality testing to the advancement of CM solutions for effective emissions mitigation.
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Monitoreo del Ambiente , Monitoreo del Ambiente/métodos , Método Simple Ciego , Metano/análisis , Contaminantes Atmosféricos/análisisRESUMEN
Quantifying and controlling fugitive methane emissions from oil and gas facilities remains essential for addressing climate goals, but the costs associated with monitoring millions of production sites remain prohibitively expensive. Current thinking, supported by measurement and simple dispersion modelling, assumes single-digit parts-per-million instrumentation is required. To investigate instrument response, the inlets of three trace-methane (sub-ppm) analyzers were collocated on a facility designed to release gas of known composition at known flow rates between 0.4 and 5.2 kg CH4 h-1 from simulated oil and gas infrastructure. Methane mixing ratios were measured by each instrument at 1 Hertz resolution over nine hours. While mixing ratios reported by a cavity ring-down spectrometer (CRDS)-based instrument were on average 10.0 ppm (range 1.8 to 83 ppm), a mid-infrared laser absorption spectroscopy (MIRA)-based instrument reported short-lived mixing ratios far larger than expected (range 1.8 to 779 ppm) with a similar nine-hour average to the CRDS (10.1 ppm). We suggest the peaks detected by the MIRA are likely caused by a micrometeorological phenomenon, where vortex shedding has resulted in heterogeneous methane plumes which only the MIRA can observe. Further analysis suggests an instrument like the MIRA (an optical-cavity-based instrument with cavity size ≤10 cm3 measuring at ≥2 Hz with air flow rates in the order of ≤0.3 slpm at distances of ≤20 m from the source) but with a higher detection limit (25 ppm) could detect enough of the high-concentration events to generate representative 20 min-average methane mixing ratios. Even though development of a lower-cost, high-precision, high-accuracy instrument with a 25 ppm detection threshold remains a significant problem, this has implications for the use of instrumentation with higher detection thresholds, resulting in the reduction in cost to measure methane emissions and providing a mechanism for the widespread deployment of effective leak detection and repair programs for all oil and gas infrastructure.
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This study evaluated multiple commercially available continuous monitoring (CM) point sensor network (PSN) solutions under single-blind controlled release testing conducted at operational upstream and midstream oil and natural gas (O&G) sites. During releases, PSNs reported site-level emission rate estimates of 0 kg/h between 38 and 86% of the time. When non-zero site-level emission rate estimates were provided, no linear correlation between the release rate and the reported emission rate estimate was observed. The average, aggregated across all PSN solutions during releases, shows 5% of the mixing ratio readings at downwind sensors were greater than the site's baseline plus two standard deviations. Four of seven total PSN solutions tested during this field campaign provided site-level emission rate estimates with the site average relative error ranging from -100% to 24% for solution D, -100% to -43% for solution E, -25% for solution F (solution F was only at one site), and -99% to 430% for solution G, with an overall average of -29% across all sites and solutions. Of all the individual site-level emission rate estimates, only 11% were within ±2.5 kg/h of the study team's best estimate of site-level emissions at the time of the releases.
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Recent studies indicate emission factors used to generate bottom-up methane inventories may have considerable regional variability. The US's Environmental Protection Agency's emission factors for plugged and unplugged abandoned oil and gas wells are largely based on measurement of historic wells and estimated at 0.4 g and 31 g CH4 well-1 h-1, respectively. To investigate if these are representative of wells more recently abandoned, methane emissions were measured from 128 plugged and 206 unplugged abandoned wells in Colorado, finding the first super-emitting abandoned well (76 kg CH4 well-1 h-1) and average emissions of 0 and 586 g CH4 well-1 h-1, respectively. Combining these with other states' measurements, we update the US emission factors to 1 and 198 g CH4 well-1 h-1, respectively. Correspondingly, annual methane emissions from the 3.4 million abandoned wells in the US are estimated at between 2.6 Tg, following current methodology, and 1.1 Tg, where emissions are disaggregated for well-type. In conclusion, this study identifies a new abandoned well-type, recently-producing orphaned, that contributes 74 % to the total abandoned wells methane emissions. Including this new well-type in the bottom-up inventory suggests abandoned well emissions equate to between 22 and 49 % of total emissions from US active oil and gas production operations.
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Studying the indoor dynamics that impact particles is crucial in order to understand indoor air chemistry and assess overall human exposure to particles. This work investigates spatial gradients in particle concentration, caused by indoor transport and loss mechanisms. We conducted a variety of cooking experiments during the House Observations of Microbial and Environmental Chemistry (HOMEChem) campaign in June 2018 that allowed us to probe these mechanisms. We measured size-resolved (0.06-1 µm and 0.13-3 µm) particle number concentrations from cooking experiments using optical instruments at four locations throughout the house simultaneously. The particle number concentration in the kitchen was 40 ± 10% and 70 ± 10% higher than the concentrations in the living room and the bedroom, respectively. There was a minor size dependence, with larger differences in the smaller sizes of the accumulation mode (0.1-2.5 µm) than the larger end of the range. Dilution accounts for the majority of these concentration differences. Surface deposition was the dominant fate of particles within a zone, with observed deposition velocities ranging from 0.1 to 0.6 m h-1.
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Contaminantes Atmosféricos , Contaminación del Aire Interior , Contaminantes Atmosféricos/análisis , Contaminación del Aire Interior/análisis , Monitoreo del Ambiente , Humanos , Tamaño de la Partícula , Material Particulado/análisisRESUMEN
Wet and dry deposition remove aerosols from the atmosphere, and these processes control aerosol lifetime and thus impact climate and air quality. Dry deposition is a significant source of aerosol uncertainty in global chemical transport and climate models. Dry deposition parameterizations in most global models were developed when few particle deposition measurements were available. However, new measurement techniques have enabled more size-resolved particle flux observations. We combined literature measurements with data that we collected over a grassland in Oklahoma and a pine forest in Colorado to develop a dry deposition parameterization. We find that relative to observations, previous parameterizations overestimated deposition of the accumulation and Aitken mode particles, and underestimated in the coarse mode. These systematic differences in observed and modeled accumulation mode particle deposition velocities are as large as an order of magnitude over terrestrial ecosystems. As accumulation mode particles form most of the cloud condensation nuclei (CCN) that influence the indirect radiative effect, this model-measurement discrepancy in dry deposition alters modeled CCN and radiative forcing. We present a revised observationally driven parameterization for regional and global aerosol models. Using this revised dry deposition scheme in the Goddard Earth Observing System (GEOS)-Chem chemical transport model, we find that global surface accumulation-mode number concentrations increase by 62% and enhance the global combined anthropogenic and natural aerosol indirect effect by -0.63 W m-2 Our observationally constrained approach should reduce the uncertainty of particle dry deposition in global chemical transport models.
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Black carbon (BC) aerosol plays an important role in the Earth's climate system because it absorbs solar radiation and therefore potentially warms the climate; however, BC can also act as a seed for cloud particles, which may offset much of its warming potential. If BC acts as an ice nucleating particle (INP), BC could affect the lifetime, albedo, and radiative properties of clouds containing both supercooled liquid water droplets and ice particles (mixed-phase clouds). Over 40% of global BC emissions are from biomass burning; however, the ability of biomass burning BC to act as an INP in mixed-phase cloud conditions is almost entirely unconstrained. To provide these observational constraints, we measured the contribution of BC to INP concentrations ([INP]) in real-world prescribed burns and wildfires. We found that BC contributes, at most, 10% to [INP] during these burns. From this, we developed a parameterization for biomass burning BC and combined it with a BC parameterization previously used for fossil fuel emissions. Applying these parameterizations to global model output, we find that the contribution of BC to potential [INP] relevant to mixed-phase clouds is â¼5% on a global average.