• Energy Research

The perfluorocarbons tetrafluoromethane (CF 4 , PFC-14) and hexafluoroethane (C 2 F 6 , PFC-116) are potent greenhouse gases with near-permanent atmospheric lifetimes relative to human timescales and global warming potentials thousands of times that of CO 2 . Using long-term atmospheric observations from a Chinese network and an inverse modeling approach (top–down method), we determined that CF 4 emissions in China increased from 4.7 (4.2-5.0, 68% uncertainty interval) Gg y −1 in 2012 to 8.3 (7.7-8.9) Gg y −1 in 2021, and C 2 F 6 emissions in China increased from 0.74 (0.66-0.80) Gg y −1 in 2011 to 1.32 (1.24-1.40) Gg y −1 in 2021, both increasing by approximately 78%. Combined emissions of CF 4 and C 2 F 6 in China reached 78 Mt CO 2 -eq in 2021. The absolute increase in emissions of each substance in China between 2011-2012 and 2017-2020 was similar to (for CF 4 ), or greater than (for C 2 F 6 ), the respective absolute increase in global emissions over the same period. Substantial CF 4 and C 2 F 6 emissions were identified in the less-populated western regions of China, probably due to emissions from the expanding aluminum industry in these resource-intensive regions. It is likely that the aluminum industry dominates CF 4 emissions in China, while the aluminum and semiconductor industries both contribute to C 2 F 6 emissions. Based on atmospheric observations, this study validates the emission magnitudes reported in national bottom–up inventories and provides insights into detailed spatial distributions and emission sources beyond what is reported in national bottom–up inventories.

AbstractWe present an analysis of methane (CH4) emissions using atmospheric observations from 13 sites in California during June 2013 to May 2014. A hierarchical Bayesian inversion method is used to estimate CH4 emissions for spatial regions (0.3° pixels for major regions) by comparing measured CH4 mixing ratios with transport model (Weather Research and Forecasting and Stochastic Time‐Inverted Lagrangian Transport) predictions based on seasonally varying California‐specific CH4 prior emission models. The transport model is assessed using a combination of meteorological and carbon monoxide (CO) measurements coupled with the gridded California Air Resources Board (CARB) CO emission inventory. The hierarchical Bayesian inversion suggests that state annual anthropogenic CH4 emissions are 2.42 ± 0.49 Tg CH4/yr (at 95% confidence), higher (1.2–1.8 times) than the current CARB inventory (1.64 Tg CH4/yr in 2013). It should be noted that undiagnosed sources of errors or uncaptured errors in the model‐measurement mismatch covariance may increase these uncertainty bounds beyond that indicated here. The CH4 emissions from the Central Valley and urban regions (San Francisco Bay and South Coast Air Basins) account for ~58% and 26% of the total posterior emissions, respectively. This study suggests that the livestock sector is likely the major contributor to the state total CH4 emissions, in agreement with CARB's inventory. Attribution to source sectors for subregions of California using additional trace gas species would further improve the quantification of California's CH4 emissions and mitigation efforts toward the California Global Warming Solutions Act of 2006 (Assembly Bill 32).

The sources of halogenated compounds in East Asia associated with stratospheric ozone depletion and climate change are relatively poorly understood. High-precision in situ measurements of 18 halogenated compounds and carbonyl sulfide (COS) made at Gosan, Jeju Island, Korea, from November 2007 to December 2011 were analyzed by a positive matrix factorization (PMF). Seven major industrial sources were identified from the enhanced concentrations of halogenated compounds observed at Gosan and corresponding concentration-based source contributions were also suggested: primary aluminum production explaining 37% of total concentration enhancements, solvent usage of which source apportionment is 25%, fugitive emissions from HCFC/HFC production with 11%, refrigerant replacements (9%), semiconductor/electronics industry (9%), foam blowing agents (6%), and fumigation (3%). Statistical trajectory analysis was applied to specify the potential emission regions for seven sources using back trajectories. Primary aluminum production, solvent usage and fugitive emission sources were mainly contributed by China. Semiconductor/electronics sources were dominantly located in Korea. Refrigerant replacement, fumigation and foam blowing agent sources were spread throughout East Asian countries. The specified potential source regions are consistent with country-based consumptions and emission patterns, verifying the PMF analysis results. The industry-based emission sources of halogenated compounds identified in this study help improve our understanding of the East Asian countries' industrial contributions to halogenated compound emissions.

Abstract. Sulfur hexafluoride (SF6) has a global warming potential of around 22 800 over a 100 yr time horizon and is one of the greenhouse gases regulated under the Kyoto Protocol. Around circa 2000 there was a reversal in the global SF6 emission trend, from a decreasing to an increasing trend, which was likely caused by increasing emissions in countries that are not obligated to report their annual emissions to the United Nations Framework Convention on Climate Change. In this study, SF6 emissions during the period 2006–2012 for all East Asian countries, including Mongolia, China, the Taiwan region, North Korea, South Korea and Japan, were determined by using inverse modeling and in-situ atmospheric measurements. We found that the most important sources of uncertainty associated with these inversions are related to the choice of a priori emissions and their assumed uncertainty, the station network as well as the meteorological input data. Much lower uncertainties are due to seasonal variability in the emissions, inversion geometry and resolution, and the measurement calibration scale. Based on the results of these sensitivity tests, we estimate that the total SF6 emission in East Asia increased rapidly from 2437 ± 329 Mg yr−1 in 2006 to 3787 ± 512 Mg yr−1 in 2009 and stabilized thereafter. China contributed 58–72 % to the total East Asian emission for the different years, followed by South Korea (9–19%), Japan (5–16%) and the Taiwan region (4–7%), while the contributions from North Korea and Mongolia together were less than 3% of the total. The per-capita SF6 emissions are highest in South Korea and the Taiwan region, while the per-capita emissions for China, North Korea and Japan are close to global average. During the period 2006–2012, emissions from China increased rapidly and emissions from South Korea increased slightly, while emissions from the Taiwan region and Japan decreased overall.