The issue of combined sewer overflow (CSO) triggered by rainfall has become a significant obstacle to the improvement of water environment quality. This study conducted a long-term monitoring of three types of rainwater outlets, i.e., combined sewer overflows (Test-CSO), separated sewer outlets (Test-SSO), and partially separated sewer outlets (Test-PSSO), to reveal the characteristics of overflow pollution and trace its sources by monitoring the pollutants from different underlying surfaces across various urban functional areas. The results showed that the major pollutants in overflow events exhibited the following order: COD ≥ TSS > TN > TAN > TP. Rainwater elevated COD and TSS in the Test-CSO, while reducing nitrogen and phosphorus concentrations by dilution. The Test-PSSO experienced varying degrees of overflow pollution, primarily due to the sewer sediment. A negative relationship between the rainfall and peak time of overflow pollution was observed. The traceability analysis indicated the overall pollution intensity exhibited the following order: residential areas > industrial parks > commercial areas. In addition to commercial areas, the pollution intensity across underlying surfaces generally exhibited the following order: roofs > roads > grasslands. The roof runoff was an important source of pollutants for overflow pollution, and TSS and COD were the major contributors. Notably, grasslands had a buffering effect on pollutants and pH.
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