Reconciling NOx emissions reductions and ozone trends in the U.S., 2002-2006

Dynamic evaluation seeks to assess the ability of photochemical models to replicate changes in air quality as emissions and other conditions change. When a model fails to replicate an observed change, a key challenge is to discern whether the discrepancy is caused by errors in meteorological simulations, errors in emission magnitudes and changes, or inaccurate responses of simulated pollutant concentrations to emission changes. In this study, the Community Multiscale Air Quality (CMAQ) model is applied to simulate the ozone (O3) change after the NOx SIP Call and mobile emission controls substantially reduced nitrogen oxides (NOx) emissions in the eastern U.S. from 2002 to 2006. For both modeled and observed O3, changes in episode average daily maximal 8-h O3 were highly correlated (R2 = 0.89) with changes in the 95th percentile, although the magnitudes of reductions increased nonlinearly at high percentile O3 concentrations. Observed downward changes in mean NOx (−11.6 to −2.5 ppb) and 8-h O3 (−10.4 to −4.7 ppb) concentrations in metropolitan areas in the NOx SIP Call region were under-predicted by 31%-64% and 26%-66%, respectively. The under-predicted O3 improvements in the NOx SIP Call region could not be explained by adjusting for temperature biases in the meteorological input, or by considering uncertainties in the chemical reaction rate constants. However, the under-prediction in O3 improvements could be alleviated by 5%-31% by constraining NOx emissions in each year based on observed NOx concentrations. This demonstrates the crucial need to accurately characterize changes in precursor emissions when dynamically evaluating a model's ability to simulate O3 responses to those changes.

► CMAQ model significantly under-predicted the observed O3 change from 2002 to 2006. ► Under-prediction of O3 change was more severe at high percentile concentrations. ► The observed NOx change was significantly underestimated in NOx SIP Call. ► Under-prediction of O3 change could be alleviated by constraining NOx emissions.