Culbertson J A, Prins J M, Grimsrud E P, Rasmussen R A, Khalil M A K, Shearer M J
Department of Chemistry and Biochemistry, Montana State University, Bozeman, MT 59717, USA.
Chemosphere. 2004 May;55(8):1109-19. doi: 10.1016/j.chemosphere.2003.11.002.
The concentrations of CF(3)-containing compounds in archived air samples collected at Cape Meares, Oregon, from 1978 to 1997, at Point Barrow, Alaska, from 1995 to 1998, and at Palmer Station, Antarctica, from 1991 to 1997, were determined by high resolution gas chromatography and high resolution mass spectrometry. The CF(3)-containing compounds measured by this method and discussed here are: the perfluorinated compound, C(3)F(8) (FC 218); four perhalogenated compounds, CF(3)Cl (CFC 13), CF(3)CF(2)Cl (CFC 115), CF(3)CFCl(2) (CFC 114a), and CF(3)Br (Halon 1301); and three hydrofluorocompounds, CF(3)H (HFC 23), CF(3)CH(3) (HFC 143a), and CF(3)CH(2)F (HFC 134a). For four of these compounds, very few measurements have been previously reported. The atmospheric concentrations of all of the CF(3)-containing compounds continuously increased in time over the sample collection periods. From these data, the annual rates of emission into the atmosphere have been estimated. The emission rates fall into one of three distinct categories. The annual emission rates of C(3)F(8), CF(3)H, CF(3)CH(3), and CF(3)CH(2)F have continuously increased over the last two decades. That of CF(3)CFCl(2) has decreased continuously. Emission rates for CF(3)Cl, CF(3)CF(2)Cl, and CF(3)Br reached maximum levels in the late 1980s, and have been decreasing in the 1990s. The emission rates of C(3)F(8), CF(3)CH(3) and CF(3)CH(2)F were nearly zero 20 years ago but have increased rapidly during the last decade.
采用高分辨率气相色谱法和高分辨率质谱法，测定了1978年至1997年在俄勒冈州梅尔斯角、1995年至1998年在阿拉斯加巴罗角以及1991年至1997年在南极洲帕尔默站采集的存档空气样本中含CF(3)化合物的浓度。通过该方法测定并在此讨论的含CF(3)化合物有：全氟化合物C(3)F(8)（FC 218）；四种全卤代化合物，CF(3)Cl（CFC 13）、CF(3)CF(2)Cl（CFC 115）、CF(3)CFCl(2)（CFC 114a）和CF(3)Br（哈龙1301）；以及三种氢氟化合物，CF(3)H（HFC 23）、CF(3)CH(3)（HFC 143a）和CF(3)CH(2)F（HFC 134a）。对于其中四种化合物，此前很少有测量报告。在样本采集期间，所有含CF(3)化合物的大气浓度均随时间持续增加。根据这些数据，估算了向大气中的年排放率。排放率分为三个不同类别之一。在过去二十年中，C(3)F(8)、CF(3)H、CF(3)CH(3)和CF(3)CH(2)F的年排放率持续增加。CF(3)CFCl(2)的年排放率持续下降。CF(3)Cl、CF(3)CF(2)Cl和CF(3)Br的排放率在20世纪80年代末达到最高水平，并在20世纪90年代有所下降。20年前，C(3)F(8)、CF(3)CH(3)和CF(3)CH(2)F的排放率几乎为零，但在过去十年中迅速增加。
