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. Comprehensive chlorine heterogeneous chemistry is incorporatedinto the Community Multiscale Air Quality (CMAQ) model to evaluate the impactof chlorine-related heterogeneous reaction on diurnal and nocturnal nitrateformation and quantify the nitrate formation from gas-to-particlepartitioning of HNO3 and from different heterogeneous pathways. Theresults show that these heterogeneous reactions increase the atmospheric Cl2 and ClNO2 level ( ∼ 100  %), which furtheraffects the nitrate formation. Sensitivity analyses of uptake coefficientsshow that the empirical uptake coefficient for the O3 heterogeneousreaction with chlorinated particles may lead to the large uncertainties inthe predicted Cl2 and nitrate concentrations. The N2O5 uptake coefficient with particulate Cl− concentration dependenceperforms better in capturing the concentration of ClNO2 and nocturnalnitrate concentration. The reaction of OH and NO2 in the daytimeincreases the nitrate by ∼15  % when the heterogeneous chlorinechemistry is incorporated, resulting in more nitrate formation from HNO3 gas-to-particle partitioning. By contrast, the contribution ofthe heterogeneous reaction of N2O5 to nitrate concentrationsdecreases by about 27 % in the nighttime, when its reactions withchlorinated particles are considered. However, the generated gas-phase ClNO2 from the heterogeneous reaction of N2O5 andchlorine-containing particles further reacts with the particle surface toincrease the nitrate by 6 %. In general, this study highlights thepotential of significant underestimation of daytime concentrations and overestimation ofnighttime nitrate concentrations for chemical transport models without properchlorine chemistry in the gas and particle phases.

Modeling the impact of heterogeneous reactions of chlorine on summertime nitrate formation in Beijing, China