In this study, tropospheric formaldehyde (HCHO) vertical column densities (VCDs) were measured using multi-axis differential optical absorption spectroscopy (MAX-DOAS) from January to November 2019 in Shenyang, Northeast China. The maximum HCHO VCD value appeared in the summer (1.74 × 10¹⁶ molec/cm²), due to increased photo-oxidation of volatile organic compounds (VOCs). HCHO concentrations increased from 08:00 and peaked near 13:00, which was mainly attributed to the increased release of isoprene from plants and enhanced photolysis at noon. The HCHO VCDs observed by MAX-DOAS and OMI have a good correlation coefficient (R) of 0.78, and the contributions from primary and secondary HCHO sources were distinguished by the multi-linear regression model. The anthropogenic emissions showed unobvious seasonal variations, and the primary HCHO was relatively stable in Shenyang. Secondary HCHO contributed 82.62%, 83.90%, 78.90%, and 41.53% to the total measured ambient HCHO during the winter, spring, summer, and autumn, respectively. We also found a good correlation (R = 0.78) between enhanced vegetation index (EVI) and HCHO VCDs, indicating that the oxidation of biogenic volatile organic compounds (BVOCs) was the main source of HCHO. The ratio of secondary HCHO to nitrogen dioxide (NO₂) was used as the tracer to analyze O₃-NO_x-VOC sensitivities. We found that the VOC-limited, VOC-NO_x-limited, and NO_x-limited regimes made up 93.67%, 6.23%, 0.11% of the overall measurements, respectively. In addition, summertime ozone (O₃) sensitivity changed from VOC-limited in the morning to VOC-NO_x-limited in the afternoon. Therefore, this study offers information on HCHO sources and corresponding O₃ production sensitivities to support strategic management decisions.

Pollutant transport has a substantial impact on the atmospheric environment in megacity clusters. However, owing to the lack of knowledge of vertical pollutant structure, quantification of transport processes and understanding of their impacts on the environment remain inadequate. In this study, we retrieved the vertical profiles of aerosols, nitrogen dioxide (NO₂), and formaldehyde (HCHO) using multi-axis differential optical absorption spectroscopy (MAX-DOAS) and analyzed three typical transport phenomena over the North China Plain (NCP) and Yangtze River Delta (YRD). We found the following: (1) the main transport layers (MTL) of aerosols, NO₂, and HCHO along the southwest–northeast transport pathway in the Jing-Jin-Ji region were approximately 400–800, 0–400, and 400–1200 m, respectively. The maximum transport flux of HCHO appeared in Wangdu (WD), and aerosol and NO₂ transport fluxes were assumed to be high in Shijiazhuang (SJZ), both urban areas being significant sources feeding regional pollutant transport pathways. (2) The NCP was affected by severe dust transport on 15 March 2021. The airborne dust suppressed dissipation and boosted pollutant accumulation, decreasing the height of high-altitude pollutant peaks. Furthermore, the dust enhanced aerosol production and accumulation, weakening light intensity. For the NO₂ levels, dust and aerosols had different effects. At the SJZ and Dongying (DY) stations, the decreased light intensity prevented NO₂ photolysis and favored NO₂ concentration increase. In contrast, dust and aerosols provided surfaces for heterogeneous reactions, resulting in reduced NO₂ levels at the Nancheng (NC) and Xianghe (XH) stations. The reduced solar radiation favored local HCHO accumulation in SJZ owing to the dominant contribution of the primary HCHO. (3) Back-and-forth transboundary transport between the NCP and YRD was found. The YRD-to-NCP and NCP-to-YRD transport processes mainly occurred in the 500–1500 and 0–1000 m layers, respectively. This transport, accompanied by the dome effect of aerosols, produced a large-scale increase in PM_2.5, further validating the haze-amplifying mechanism.

Persistent heavy haze episodes have repeatedly shrouded North China in recent years. Besides anthropogenic emissions, natural dust also contributes to the aerosols in this region. Through continuous observation by a dual-wavelength Raman lidar, the primary aerosol types and their contributions to air pollution in North China were determined. The following three aerosol types can be classified: natural dust, anthropogenic aerosols, and the mixture of anthropogenic aerosols and dust (polluted dust). The classification results are basically consistent with the classification results from the cloud–aerosol lidar and infrared pathfinder satellite observations (CALIPSO) satellite measurements. The relative bias of the lidar ratio between the Raman lidar and CALIPSO is less than 25% over 90% of the cases, indicating that the CALIPSO lidar ratio selection algorithm is reasonable. The classification results show that approximately 45% of aerosols below 1.8 km are contributed by polluted dust during our one year observations. The contribution of dust increased with height, from 6% at 500 m to 28% at 1,800 m, while the contribution of anthropogenic aerosols decreased from 49% to 25%. In addition, polluted dust is the major aerosol subtype below 1.0 km in spring (over 60%) and autumn (over 70%). Anthropogenic aerosols contribute more than 75% of air pollution in summer. In winter, anthropogenic aerosols prevailed (over 80%) in the lower layer, while polluted dust (around 60%) dominated the upper layer. Our results identified the primarily aerosol types to assess the contributions of anthropogenic and natural sources to air pollution in North China, and highlight that natural dust plays a crucial role in lower-layer air pollution in spring and autumn, while controlling anthropogenic aerosols will significantly improve air quality in winter.