This study proposes a novel two-step deep learning (DL) model for estimating surface NO2 concentrations using satellite data over the contiguous United States (CONUS) from 2005 to 2019. The first phase of the model uses partial convolutional neural network (PCNN), an advanced DL model that accurately imputes gaps between surface NO2 stations and creates 5,478 daily-mean NO2 grids (PCNN-NO2) of the 2005–2019 period over the study area. We then feed the PCNN-NO2, along with other predictor variables, into a deep neural network (DNN) to estimate surface NO2 levels, achieving exceptional performance with a correlation coefficient of 0.975–0.978, a mean absolute bias of 0.99–1.38 ppb, and a root mean square error of 1.47–1.97 ppb. Spatial cross-validation results also indicate strong spatial performance of PCNN-DNN surface NO2 estimates. In addition to its accurate estimates, the PCNN-DNN model consistently generates estimated NO2 grids without any missing values, improving the quality of various applications such as emission reduction strategies and public health studies. Between 2005 and 2019, the 5,478 daily estimated NO2 grids over the CONUS reveal significant reductions in NO2 levels in 14 major urban environments: Washington D.C. (−43%), New York (−45%), Los Angeles (−38%), Chicago (−25%), Boston (−43%), Houston (−34%), Dallas (−40%), Philadelphia (−41%), Phoenix (−38%), Detroit (−20%), Denver (−23%), Atlanta (−0.7%), Cincinnati (−38%), and Pittsburgh (−56%). Furthermore, the study shows that the denser urban regions that in-situ stations are installed in, the higher the difference between in-situ observations and regional-mean NO2 levels
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