Towards sector-based attribution using intra-city variations in satellite-based emission ratios between CO₂ and CO

Abstract

Carbon dioxide (CO2) and air pollutants such as carbon monoxide (CO) are co-emitted by many combustion sources. Previous efforts have combined satellite-based observations of multiple tracers to calculate their emission ratio (ER) for inferring combustion efficiency at the regional to city scale. Very few studies have focused on combustion efficiency at the sub-city scale or related it to emission sectors using space-based observations. Several factors are important for interpreting and deriving spatially resolved ERs from asynchronous satellite measurements, including (1) variations in meteorological conditions given the mismatch in satellite overpass times, (2) differences in vertical sensitivity of the retrievals (i.e., averaging kernel profiles), (3) interferences from the biosphere and biomass burning, and (4) the mismatch in the daytime variations of CO and CO2 emissions. In this study, we extended an established emission estimate approach to arrive at spatially resolved ERs based on retrieved column-averaged CO2 (XCO2) from the Snapshot Area Mapping (SAM) mode of the Orbiting Carbon Observatory-3 (OCO-3) and column-averaged CO from the TROPOspheric Monitoring Instrument (TROPOMI). To evaluate the influences of the confounding factors listed above and further attribute intra-urban variations in ERs to certain sectors, we leveraged a Lagrangian atmospheric transport model with an urban land cover classification dataset and reported ERCO values from the sounding level to the overpass and city level. We found that the differences in overpass times and averaging kernels between OCO and TROPOMI strongly affect the estimated spatially resolved ERCO. Specifically, a time difference of >3 h typically led to dramatic changes in wind directions and urban plume shapes, thereby making the calculation of accurate sounding-specific ERCO difficult. After removing such cases from consideration and applying a simple plume shift method when necessary to account for changes in wind direction and speed, we discovered significant contrasts in combustion efficiencies between (1) two megacities versus two industry-oriented cities and (2) different regions within a city, based on six nearly coincident overpasses per city. Results suggest that the ERCO impacted by heavy industry in Los Angeles is slightly lower than the overall city-wide value (<10 ppb-CO/ppm-CO2). In contrast, the ERCO related to heavy industry in Shanghai is much higher than Shanghai's city mean and more aligned with the city means of two selected industry-oriented cities in China (approaching 20 ppb-CO/ppm-CO2). Although investigations based on a larger number of satellite overpasses are needed, our unique approach (i.e., without using sector-specific information from emission inventories) provides new insights into assessing combustion efficiency within a city from future satellite missions, such as those that will map column CO2 and CO concentrations simultaneously with high spatiotemporal resolutions.