ABSTRACT

Fine particle (PM_2.5) exposure is a public health issue affecting millions of people worldwide. In New York State, significant emission reductions occurred during the past decades due to fuel switching, increased renewable energy, and transformations in buildings and transportation. Between 2002 and 2018, anthropogenic emissions of CO, NO_x, SO₂, VOCs, and primary PM_2.5 declined by 58%, 61%, 89%, 47%, and 29%, respectively, in New York and three adjoining states. Ambient PM_2.5 mass concentrations decreased but contributions of source types to changes in PM_2.5 elemental carbon (EC) and organic carbon (OC) are incompletely understood. Receptor modeling was used to estimate changing source contributions to EC and OC in New York City (NYC) between 2007 and 2019. Source identification was facilitated by incorporating measurements of CO, NO, NO₂, O₃, SO_2, and speciated hydrocarbons (1,3-butadiene, n-butane, isobutane, n-pentane, isopentane, isoprene, benzene, toluene, xylenes, acetaldehyde, and formaldehyde). Hydrocarbon species identified mobile-source emissions, evaporative emissions, biogenics, and photochemical secondary organic aerosol. At three study locations, predicted reductions of TC (OC + EC) summed over all source types were 1.3 ± 0.2 μg m⁻³, compared with a measured TC reduction of 1.5 ± 0.2 μg m⁻³. Declining sulfate concentrations and cleaner mobile sources together reduced the predicted average TC by a combined 1 μg m⁻³. Smaller changes occurred in other source contributions, e.g., 0.15 ± 0.01 μg m⁻³ reduction likely in response to NYC regulations related to heating fuel oil. Biomass burning PM_2.5 increased between 2007 and 2011, then declined between 2015 and 2019. Reductions contrast with a non-significant increase of 0.05 μg m⁻³ in photochemical TC. Further opportunities to decrease PM_2.5 concentrations include wood burning and photochemical-related OC. Continued temporal analysis and source apportionment will be needed to track changes in air quality and source contributions as jurisdictions expand renewable energy and energy efficiency goals.

Implications: Large emission reductions that occurred in the eastern U.S. between 2002 and 2019 lowered average fine particle concentrations in New York City by a factor of two. Secondary organic aerosol concentrations declined as sulfate decreased but increased non-significantly with rising ozone. Cleaner mobile-source emissions lowered elemental and organic carbon concentrations. Opportunities for further reductions of PM_2.5 concentrations include biomass burning and photochemical secondary aerosol.

摘要

细颗粒物 (PM _2.5 ) 暴露是影响全球数百万人的公共卫生问题。在纽约州，由于燃料转换、可再生能源的增加以及建筑和交通的转型，过去几十年的排放量显着减少。2002 年至 2018 年间，纽约和三个相邻州的 CO、NO _x、SO ₂、VOC 和初级 PM _{2.5 的}人为排放量分别下降了 58%、61%、89%、47% 和 29%。环境 PM _2.5质量浓度下降，但源类型对 PM _2.5变化的贡献元素碳 (EC) 和有机碳 (OC) 尚未完全了解。受体模型用于估计 2007 年至 2019 年期间纽约市 (NYC) 对 EC 和 OC 的变化源贡献。通过结合对 CO、NO、NO ₂、O ₃、SO ₂和特定碳氢化合物的测量来促进源识别（ 1,3-丁二烯、正丁烷、异丁烷、正戊烷、异戊烷、异戊二烯、苯、甲苯、二甲苯、乙醛和甲醛）。烃类确定了移动源排放、蒸发排放、生物成因和光化学二次有机气溶胶。在三个研究地点，所有源类型总和的 TC (OC + EC) 预测减少量为 1.3 ± 0.2 μg m ^-3，与测得的 TC 减少 1.5 ± 0.2 μg m ^{-3 相比}。下降的硫酸盐浓度和更清洁的移动源共同使预测的平均 TC 减少了 1 μg m ^-3。其他来源的贡献发生了较小的变化，例如，0.15 ± 0.01 μg m ^-3减少可能是响应纽约市与加热燃料油相关的法规。生物质燃烧 PM _2.5在 2007 年和 2011 年之间增加，然后在 2015 年和 2019 年之间下降。减少与光化学 TC中 0.05 μg m ^-3的非显着增加形成对比。进一步降低 PM _{2.5 的}机会浓度包括木材燃烧和光化学相关的 OC。随着司法管辖区扩大可再生能源和能源效率目标，将需要持续的时间分析和源分配来跟踪空气质量和源贡献的变化。

影响：2002 年至 2019 年期间美国东部发生的大规模减排使纽约市的平均细颗粒浓度降低了两倍。二次有机气溶胶浓度随着硫酸盐的减少而下降，但随着臭氧的升高而增加不显着。更清洁的移动源排放降低了元素和有机碳的浓度。进一步降低 PM _2.5浓度的机会包括生物质燃烧和光化学二次气溶胶。