Unexpected nascent atmospheric emissions of three ozone-depleting hydrochlorofluorocarbons.

Global and regional atmospheric measurements and modeling can play key roles in discovering and quantifying unexpected nascent emissions of environmentally important substances. We focus here on three hydrochlorofluorocarbons (HCFCs) that are restricted by the Montreal Protocol because of their roles in stratospheric ozone depletion. Based on measurements of archived air samples and on in situ measurements at stations of the Advanced Global Atmospheric Gases Experiment (AGAGE) network, we report global abundances, trends, and regional enhancements for HCFC-132b ([Formula: see text]), which is newly discovered in the atmosphere, and updated results for HCFC-133a ([Formula: see text]) and HCFC-31 ([Formula: see text]ClF). No purposeful end-use is known for any of these compounds. We find that HCFC-132b appeared in the atmosphere 20 y ago and that its global emissions increased to 1.1 Gg⋅y-1 by 2019. Regional top-down emission estimates for East Asia, based on high-frequency measurements for 2016-2019, account for ∼95% of the global HCFC-132b emissions and for ∼80% of the global HCFC-133a emissions of 2.3 Gg⋅y-1 during this period. Global emissions of HCFC-31 for the same period are 0.71 Gg⋅y-1 Small European emissions of HCFC-132b and HCFC-133a, found in southeastern France, ceased in early 2017 when a fluorocarbon production facility in that area closed. Although unreported emissive end-uses cannot be ruled out, all three compounds are most likely emitted as intermediate by-products in chemical production pathways. Identification of harmful emissions to the atmosphere at an early stage can guide the effective development of global and regional environmental policy.

Reconciling reported and unreported HFC emissions with atmospheric observations.

We infer global and regional emissions of five of the most abundant hydrofluorocarbons (HFCs) using atmospheric measurements from the Advanced Global Atmospheric Gases Experiment and the National Institute for Environmental Studies, Japan, networks. We find that the total CO2-equivalent emissions of the five HFCs from countries that are required to provide detailed, annual reports to the United Nations Framework Convention on Climate Change (UNFCCC) increased from 198 (175-221) Tg-CO2-eq ⋅ y(-1) in 2007 to 275 (246-304) Tg-CO2-eq ⋅ y(-1) in 2012. These global warming potential-weighted aggregated emissions agree well with those reported to the UNFCCC throughout this period and indicate that the gap between reported emissions and global HFC emissions derived from atmospheric trends is almost entirely due to emissions from nonreporting countries. However, our measurement-based estimates of individual HFC species suggest that emissions, from reporting countries, of the most abundant HFC, HFC-134a, were only 79% (63-95%) of the UNFCCC inventory total, while other HFC emissions were significantly greater than the reported values. These results suggest that there are inaccuracies in the reporting methods for individual HFCs, which appear to cancel when aggregated together.

Atmospheric methane at Zeppelin Station in Ny-Alesund: presentation and analysis of in situ measurements.

In situ methane (CH(4)) measurement techniques and data from the Zeppelin Station in Ny-Alesund on Svalbard (N 78 degrees 54' E 11 degrees 53') on Mt. Zeppelin (475 m.a.s.l) are presented. The data span the time period from October 1998 to December 2003, though not continuously. The daily mean was calculated from 96 samples per day which are analysed by gas chromatography with flame ionisation detection. Details of the experimental methods and procedures are given. A harmonic function is fitted to the data with a constant trend and seasonal amplitude. The data are also presented in a regression plot showing the difference between the in situ measurements and flask measurements from the National Oceanic and Atmospheric Administration of the Climate Monitoring and Diagnostics Laboratory (NOAA/CMDL) in Boulder, Colorado (http://www.cmdl.noaa.gov/). The Zeppelin data show typical Arctic air characteristics with wintertime pollution episodes from Europe and Russia and a relatively calm summer state.

A tracer method for evaluating recirculation of pollutant releases in buildings.

A method is introduced for evaluating recirculation in a building ventilation system from pollutant emissions in or near the building. Tracer was released at a known rate at the point of pollutant emission. Using measured tracer concentrations, the tracer release rate, and an estimate of the pollutant release rate, pollutant concentrations were estimated at the locations in the building where the tracer was measured. The method can be used to test whether a ventilation system is adequate for maintaining an acceptable work environment before work with a hazardous substance begins. In a case study presented to illustrate the technique, initial attempts to correct a problem of recirculation of sulfuric acid from a fume hood in a chemistry laboratory were shown to be inadequate, prompting the ventilation contractor to make further repairs before work with sulfuric acid could be resumed.