Long-Term Multivariate Screening of a Recirculating Landfill Leachate Circuit: Pollutant Dynamics, Statistical Structure and Associated Risk to Biota

Abstract

Landfill leachate circuits that operate without discharge, by recirculating aerated leachate onto the waste mass, are widespread in South-East Europe, yet their long-term behaviour is rarely documented with sample-level data. This study reports a six-year (2020–2025) seasonal monitoring campaign at a sanitary landfill in northern Serbia (alluvial aquifer of the Sava River, transboundary Danube basin) and re-examines it with a transparent multivariate protocol. Seventy-two leachate samples (collection well, aeration lagoon, sedimentation lagoon; n = 24 each, 30 parameters), 28 realised surface-water campaigns, and six years of groundwater summaries were evaluated by principal component analysis/factor analysis (PCA/FA, Varimax normalized), hierarchical cluster analysis, PERMANOVA, non-parametric paired tests and, for benchmarking, supervised machine learning. The pooled leachate model (n = 72; 21 variables; KMO = 0.700; Bartlett χ2 = 956, p < 0.001) retained four factors by parallel analysis, explaining 61.6% of total variance; after rotation the factors accounted for 27.7%, 14.3%, 10.4%, and 9.3%. Factor 1 grouped organic load with particle-reactive metals (COD, BOD5, Fe, Ni, Cr, As, Zn), Factor 2 a reduced sulfur–fluoride–BTEX signature, Factor 3 temperature-driven nitritation, and Factor 4 a nitrate–manganese redox contrast. Crucially, paired campaign-by-campaign comparison showed no removal of the dominant pollutants along the circuit. Median COD, BOD5 and NH4-N were not lower in the sedimentation lagoon than in the collection well, while pH rose from 8.08 to 8.75 (p < 0.001); only Cu, Pb, NO3-N, and NO2-N decreased significantly. The circuit therefore homogenises and concentrates dissolved load rather than removing it. Downstream surface water was significantly enriched in electrical conductivity (+110 µS/cm), total dissolved solids, NH4-N, and NO2-N relative to upstream (Wilcoxon, p < 0.05), and groundwater showed episodic conductivity up to 12,760 µS/cm and NH4-N up to 102 mg/L. Cytotoxicity (MTT) confirmed biological relevance, with MRC-5 viability falling to 37% after 24 h exposure to 50 vol.% groundwater (Pw3) versus 60% in A549 cells. A random-forest classifier separated circuit units far better than PCA-based discrimination (76.4% versus 54.2% cross-validated accuracy) and distinguished the 2020–2021 pandemic period from 2022–2025 with 94.2% accuracy, a period effect also confirmed by PERMANOVA (R2 = 7.2%, p < 0.001). The results indicate that closed-loop recirculation without an engineered discharge barrier transfers, rather than eliminates, contaminant load, and that after-care of such systems requires mass-balance monitoring and polishing treatment.