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Attribution of Tropospheric Ozone to NOₓ and VOC Emissions: Considering Ozone Formation in the Transition Regime

Author:
Wang, Peng, Chen, Yuan, Hu, Jianlin, Zhang, Hongliang, Ying, Qi
Source:
Environmental science & technology 2018 v.53 no.3 pp. 1404-1412
ISSN:
1520-5851
Subject:
air pollution, air quality, emissions, hydrogen peroxide, hydroperoxides, issues and policy, models, nitric acid, nitrogen oxides, ozone, river deltas, rivers, troposphere, volatile organic compounds, China, Yangtze River
Abstract:
An improved three-regime (3R) O₃ attribution technique for O₃ source apportionment in regional chemical transport models is developed to divide the entire range of VOC-NOₓ-O₃ formation sensitivity to VOC-limited, transition, and NOₓ-limited regimes based on the value of a regime indicator R. The threshold R values to mark the start (Rₜₛ) and end (Rₜₑ) of the transition regime are defined at the point where O₃–NOₓ sensitivity turns from negative to positive and where O₃–NOₓ sensitivity is ten times higher than O₃–VOC sensitivity, respectively. Rₜₛ and Rₜₑ are determined using NOₓ and VOC sensitivity simulations in a box model with a modified SAPRC-11 mechanism. For the widely used indicator ration R = (PH₂O₂ + PROOH)/PHNO₃, which is based on the production rates of H₂O₂, HNO₃ and organic hydroperoxides (ROOH), the recommended Rₜₛ and Rₜₑ values are 0.047 and 5.142, respectively. Parameterized attribution functions, depending only on the values of R, are developed to apportion modeled in situ O₃ formation in the transition regime to NOₓ and VOCs. The new 3R and the traditional two-regime (2R) schemes are incorporated into the Community Multiscale Air Quality (CMAQ) model to quantify NOₓ and VOC contributions to regional O₃ concentrations in China in August 2013. The 3R approach predicts approximately 5–10 ppb and up to 15 ppb higher NOₓ contributions to 8 h O₃ in in the North China Plain, the Yangtze River Delta and the Pearl River Delta than the 2R approach. The big differences in O₃ attribution between 2R and 3R can have significant policy implications for air pollution emission controls.
Agid:
6300716