Atmospheric Chemistry and Physics. 16:365-382.
High frequency, in situ observations from 11 globally distributed sites for the period 1994-2014 and archived air measurements dating from 1978 onward have been used to determine the global growth rate of 1,1-difluoroethane (HFC-152a, CH3CHF2). These observations have been combined with a range of atmospheric transport models to derive global emission estimates in a top-down approach. HFC-152a is a greenhouse gas with a short atmospheric lifetime of about 1.5 years. Since it does not contain chlorine or bromine, HFC-152a makes no direct contribution to the destruction of stratospheric ozone and is therefore used as a substitute for the ozone de- pleting chlorofluorocarbons (CFCs) and hydrochlorofluorocarbons (HCFCs). The concentration of HFC-152a has grown substantially since the first direct measurements in 1994, reaching a maximum annual global growth rate of 0.84 +/- 0.05 ppt yr(-1) in 2006, implying a substantial increase in emissions up to 2006. However, since 2007, the annual rate of growth has slowed to 0.38 +/- 0.04 ppt yr(-1) in 2010 with a further decline to an annual average rate of growth in 2013-2014 of -0.06 +/- 0.05 ppt yr(-1). The annual average Northern Hemisphere (NH) mole fraction in 1994 was 1.2 ppt rising to an annual average mole fraction of 10.1 ppt in 2014. Average annual mole fractions in the Southern Hemisphere (SH) in 1998 and 2014 were 0.84 and 4.5 ppt, respectively. We estimate global emissions of HFC-152a have risen from 7.3 +/- 5.6 Gg yr(-1) in 1994 to a maximum of 54.4 +/- 17.1 Gg yr(-1) in 2011, declining to 52.5 +/- 20.1 Gg yr(-1) in 2014 or 7.2 +/- 2.8 Tg-CO2 eq yr(-1). Analysis of mole fraction enhancements above regional background atmospheric levels suggests substantial emissions from North America, Asia, and Europe. Global HFC emissions (so called "bottom up" emissions) reported by the United Nations Framework Convention on Climate Change (UNFCCC) are based on cumulative national emission data reported to the UNFCCC, which in turn are based on national consumption data. There appears to be a significant underestimate (> 20 Gg) of "bottom-up" reported emissions of HFC-152a, possibly arising from largely underestimated USA emissions and undeclared Asian emissions.