Parrish David D, Faloona Ian C, Derwent Richard G
Air Quality Research Center, University of California, Davis, California, USA.
David.D.Parrish, LLC, Boulder, Corolado, USA.
J Air Waste Manag Assoc. 2022 May;72(5):434-454. doi: 10.1080/10962247.2022.2050962. Epub 2022 Apr 7.
Archived Ozone Design Values (ODVs) provide smoothed temporal records of maximum ozone concentrations impacting monitoring sites throughout the US. Utilizing time series of ODVs recorded at sites along the US West Coast, we separately estimate ODV contributions from US background ozone and from production driven by US anthropogenic precursor emissions. Sondes launched from Trinidad Head in northern California measure the vertical distribution of baseline ozone transported ashore from the Pacific; this profile is reflected in the increase of the US background ODV contribution with monitoring site elevation in both rural and urban areas. The ODVs that would result from US background ozone alone are small at coastal, sea level locations (average 45 ppb), but increase with altitude; above 1 km US background ODVs can exceed 60 ppb. US background ozone contributions now constitute the majority of the maximum ODVs throughout the US west coast region, including the Los Angeles urban area, which records the country's highest ODVs. US anthropogenic emissions presently cause enhancements of 35 to 55 ppb to the maximum ODVs in the Los Angeles area; thus, local emission controls can further reduce ozone even though the background contribution is larger. In other US west coast urban areas ODV enhancements from US anthropogenic emissions are much smaller than the US background ODV contribution. The past decrease in US anthropogenic ODV enhancements from emission controls is larger than generally realized - a factor of more than 6 from 1980 to 2020, while US background ODV contributions varied to only a small extent over those four decades. Wildfire impacts on ODVs are significant in urban areas of the Pacific Northwest, but not over the vast northern US rural region. There is an indication that agricultural emissions of nitrogen oxides in California's Salinas Valley increase downwind maximum ODVs by 5-10 ppb.: In 2020 the ozone design values (ODVs) resulting from transported background ozone alone are now larger than the ODV enhancements from US anthropogenic precursor emissions, even in the Los Angeles urban area, where the nation's highest ODVs are recorded. The US anthropogenic ODV enhancements have been reduced by more than a factor of 6 from 1980 to 2020. The maximum US background ODV contributions have varied somewhat, but in each of the US west coast urban areas it was 60 ppb or larger in 2000. These contributions are so large that reducing maximum urban ODVs to the 70 ppb required by the 2015 ozone NAAQS is very difficult. There remains relatively little room for further reducing ODVs through domestic emission controls alone. From this perspective, degraded US ozone air quality in the western US is primarily due to the US background ozone contribution, with the US anthropogenic enhancement making a significant, but smaller contribution. Notably, the US background ODV has slowly decreased (1 ppb decade; Parrish, Derwent, and Faloona 2021) since the mid-2000s; cooperative, international emission control efforts aimed at continuing or even accelerating this background ozone decrease may be an effective approach to further ODV reductions, since the US background ODV is largely due to a hemisphere-wide, transported reservoir of ozone with contributions from all northern midlatitude continents. Given the major contribution of background ozone to observed ODVs, future reviews of the ozone NAAQS will be better informed if observational-based estimates of background ODV contributions are considered, in addition to model-derived estimates upon which past reviews have solely relied.
存档的臭氧设计值(ODV)提供了影响美国各地监测站点的最大臭氧浓度的平滑时间记录。利用美国西海岸沿线站点记录的ODV时间序列,我们分别估算了美国背景臭氧以及美国人为前体排放驱动产生的臭氧对ODV的贡献。从加利福尼亚州北部的特立尼达角发射的探空仪测量了从太平洋输送到岸上的基线臭氧的垂直分布;这种分布情况反映在美国背景ODV贡献随着农村和城市地区监测站点海拔的升高而增加。仅由美国背景臭氧产生的ODV在沿海海平面位置较小(平均约45 ppb),但会随着海拔升高而增加;在海拔1公里以上,美国背景ODV可能超过60 ppb。目前,美国背景臭氧贡献在整个美国西海岸地区,包括记录了美国最高ODV的洛杉矶市区,构成了最大ODV的大部分。目前,美国人为排放使洛杉矶地区的最大ODV增加了35至55 ppb;因此,即使背景贡献更大,当地的排放控制措施仍可进一步降低臭氧浓度。在美国西海岸的其他城市地区,美国人为排放导致的ODV增加远小于美国背景ODV贡献。过去,排放控制措施使美国人为ODV增加量减少的幅度比一般认识的要大——从1980年到2020年超过了6倍,而在这四十年里,美国背景ODV贡献仅在很小的范围内变化。野火对ODV的影响在太平洋西北部的城市地区较为显著,但在美国北部广大农村地区则不明显。有迹象表明,加利福尼亚州萨利纳斯山谷的农业氮氧化物排放使下风向的最大ODV增加了5 - 10 ppb。:2020年,仅由输送来的背景臭氧产生的臭氧设计值(ODV)现在大于美国人为前体排放导致的ODV增加量,即使在记录了美国最高ODV的洛杉矶市区也是如此。从1980年到2020年,美国人为ODV增加量减少了超过6倍。美国背景ODV的最大贡献有所变化,但在2000年美国西海岸的每个城市地区,其值都达到了60 ppb或更高。这些贡献如此之大,以至于将城市最大ODV降至2015年臭氧国家环境空气质量标准(NAAQS)要求的70 ppb非常困难。仅通过国内排放控制进一步降低ODV的空间相对较小。从这个角度来看,美国西部臭氧空气质量下降主要归因于美国背景臭氧贡献,美国人为排放的增加虽有显著影响,但占比相对较小。值得注意的是,自21世纪中叶以来,美国背景ODV已缓慢下降(约1 ppb/十年;帕里什、德温特和法卢纳,2021年);旨在持续甚至加速这种背景臭氧下降的合作性国际排放控制努力可能是进一步降低ODV的有效途径,因为美国背景ODV很大程度上归因于半球范围内输送的臭氧库,所有北半球中纬度大陆都对其有贡献。鉴于背景臭氧对观测到的ODV有主要贡献,除了过去评估仅依赖的模型推导估计值外,如果考虑基于观测的背景ODV贡献估计值,未来对臭氧NAAQS的审查将更有依据。