A meteorologically adjusted ensemble Kalman filter approach for inversing daily emissions:A case study in the Pearl River Delta,China

The conventional Ensemble Kalman filter(EnKF),which is now widely used to calibrate emission inventories and to improve air quality simulations,is susceptible to simulation errors of meteorological inputs,making accurate updates of high temporal-resolution emission inventories challenging.In this study,we developed a novel meteorologically adjusted inversion method(MAEInv)based on the EnKF to improve daily emission estimations.The new method combines sensitivity analysis and bias correction to alleviate the inversion biases caused by errors of meteorological inputs.For demonstration,we used the MAEInv to inverse daily carbon monoxide(CO)emissions in the Pearl River Delta(PRD)region,China.In the case study,60%of the total CO simulation biases were associated with sensitive meteorological inputs,which would lead to the overestimation of daily variations of posterior emissions.Using the new inversion method,daily variations of emissions shrank dramatically,with the percentage change decreased by 30%.Also,the total amount of posterior CO emissions estimated by the MAEInv decreased by 14%,indicating that posterior CO emissions might be overestimated using the conventional EnKF.Model evaluations using independent observations revealed that daily CO emissions estimated by MAEInv better reproduce the magnitude and temporal patterns of ambient CO concentration,with a higher correlation coefficient(R,+37.0%)and lower normalized mean bias(NMB,-17.9%).Since errors of meteorological inputs are major sources of simulation biases for both low-reactive and reactive pollutants,the MAEInv is also applicable to improve the daily emission inversions of reactive pollutants.

Impacts of meteorology and precursor emission change on O_(3) variation in Tianjin, China from 2015 to 2021

Deterioration of surface ozone (O_(3)) pollution in Northern China over the past few years received much attention.For many cities,it is still under debate whether the trend of surface O_(3)variation is driven by meteorology or the change in precursors emissions.In this work,a time series decomposition method (Seasonal-Trend decomposition procedure based on Loess (STL)) and random forest (RF) algorithm were utilized to quantify the meteorological impacts on the recorded O_(3)trend and identify the key meteorological factors affecting O_(3)pollution in Tianjin,the biggest coastal port city in Northern China.After “removing” the meteorological fluctuations from the observed O_(3)time series,we found that variation of O_(3)in Tianjin was largely driven by the changes in precursors emissions.The meteorology was unfavorable for O_(3)pollution in period of 2015-2016,and turned out to be favorable during 2017-2021.Specifically,meteorology contributed 9.3μg/m^(3)O_(3)(13%) in 2019,together with the increase in precursors emissions,making 2019 to be the worst year of O_(3)pollution since 2015.Since then,the favorable effects of meteorology on O_(3)pollution tended to be weaker.Temperature was the most important factor affecting O_(3)level,followed by air humidity in O_(3)pollution season.In the midday of summer days,O_(3)pollution frequently exceeded the standard level (>160μg/m^(3)) at a combined condition with relative humidity in 40%-50%and temperature>31℃.Both the temperature and the dryness of the atmosphere need to be subtly considered for summer O_(3)forecasting.