短寿命卤素在历史时期全球大气氧化中的关键作用。

IF 3.5 Q3 ENVIRONMENTAL SCIENCES
Adriana Bossolasco, Rafael P. Fernandez, Qinyi Li, Anoop S. Mahajan, Julián Villamayor, Javier A. Barrera, Dwayne E. Heard, Carlos A. Cuevas, Cyril Caram, Sophie Szopa and Alfonso Saiz-Lopez
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引用次数: 0

摘要

大气氧化在很大程度上决定了甲烷、臭氧和气溶胶等短期气候因子的丰度和寿命,也决定了大气中污染物的清除。羟基、硝酸盐和氯自由基(OH、NO3和Cl)以及臭氧(O3)是主要的大气氧化剂。短寿命卤素(SLH)通过直接化学反应或通过干扰其主要来源和汇间接影响这些氧化剂的浓度。然而,在历史时期,SLH对全球氧化剂的综合丰度的影响仍然没有量化,也没有在空气质量和气候模型中考虑。在这里,我们采用最先进的化学-气候模型来全面评估SLH在工业化前(PI)和现代(PD)条件下对大气氧化的作用。我们的研究结果表明,由slh驱动的全球边界层OH(16%)、NO3(38%)和臭氧(26%)水平的联合减少导致了当今大气氧化的大幅减少,而Cl的显著增加(2632%)并未补偿这一减少。这些大气氧化剂的全球差异表现出很大的空间异质性,这是由于SLH排放的变异性及其与人为污染的非线性化学相互作用。值得注意的是,我们发现SLH的作用在原始PI大气中更为明显,其中四分之一(OH: -25%)和一半(NO3: -49%)的主要白天和夜间大气氧化剂的边界层浓度分别受SLH化学控制。由于模式中没有包含slh介导的全球大气氧化的实质性减少,可能导致在过去和现在计算大气氧化能力、短期气候强迫因子和污染物的浓度和趋势时出现重大误差。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Key role of short-lived halogens on global atmospheric oxidation during historical periods†

Key role of short-lived halogens on global atmospheric oxidation during historical periods†

Atmospheric oxidation largely determines the abundance and lifetime of short-lived climate forcers like methane, ozone and aerosols, as well as the removal of pollutants from the atmosphere. Hydroxyl, nitrate and chlorine radicals (OH, NO3 and Cl), together with ozone (O3), are the main atmospheric oxidants. Short-lived halogens (SLH) affect the concentrations of these oxidants, either through direct chemical reactions or indirectly by perturbing their main sources and sinks. However, the effect of SLH on the combined abundance of global oxidants during historical periods remains unquantified and is not accounted for in air quality and climate models. Here, we employ a state-of-the-art chemistry–climate model to comprehensively assess the role of SLH on atmospheric oxidation under both pre-industrial (PI) and present-day (PD) conditions. Our results show a substantial reduction in present-day atmospheric oxidation caused by the SLH-driven combined reduction in the global boundary layer levels of OH (16%), NO3 (38%) and ozone (26%), which is not compensated by the pronounced increase in Cl (2632%). These global differences in atmospheric oxidants show large spatial heterogeneity due to the variability in SLH emissions and their nonlinear chemical interactions with anthropogenic pollution. Remarkably, we find that the effect of SLH was more pronounced in the pristine PI atmosphere, where a quarter (OH: −25%) and half (NO3: −49%) of the boundary layer concentration of the main daytime and nighttime atmospheric oxidants, respectively, were controlled by SLH chemistry. The lack of inclusion of the substantial SLH-mediated reduction in global atmospheric oxidation in models may lead to significant errors in calculations of atmospheric oxidation capacity, and the concentrations and trends of short-lived climate forcers and pollutants, both historically and at present.

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