Supplementation of tea polyphenols in sludge Fenton oxidation improves sludge dewaterability and reduces chemicals consumption

• A novel tea polyphenols (TP) mediated Fenton system was used for sludge dewatering • TP-Fenton system improved sludge dewatering at pH 7.5 and halved Fe 2+ /H 2 O 2 usage • TP could bond readily with Fe 3+ /Fe 2+ at neutral pH to form stable Fe-complexes • TP-Fenton system boosted conversion of Fe 3+ to Fe 2+ to yield more •OH in sludge • Macromolecular exopolymers degradation and cell lysis favoured sludge dewatering The Fenton oxidation improves sludge dewatering but faces notable technical and economic challenges, including a narrow acidic pH range, slow reduction of Fe(III), and the use of high doses of chemicals. Herein, we used a natural polyhydroxyphenol tea polyphenols (TP), as an iron redox conversion enhancer, to mitigate these issues. Compared with the classical Fenton process at pH 3.0, the process with TP (33.8 mg/g dry solids (DS)) improved sludge dewaterability at pH 7.5 in a Fenton-like system with faster Fe(II)/Fe(III) cycling and two times lower consumption of the Fenton reagent. Sludge capillary suction time and specific resistance to filtration decreased from 70 s to 22 s and from 2.7 × 10 13 m/kg to 5.2 × 10 11 m/kg, respectively, while the required doses of Fe(II) and H 2 O 2 were cut to 25 mg/g DS and 31.2 mg/g DS. Mechanistically, TP could bond readily with Fe(II)/Fe(III) at neutral pH to form stable complexes with complexation constants of 34 ± 161 M −1 and 52 ± 70 M −1 , respectively, and reduce part of the Fe(III) to Fe(II) simultaneously. This maintained sufficient soluble Fe in the sludge and boosted efficient conversion of Fe(II)/Fe(III) to yield more hydroxyl radicals (•OH). Subsequently, •OH oxidation resulted in the decomposition of biopolymers with a molecular weight of 10 8 Da (e.g., 58.2% of polysaccharides and 31.6% of proteins in tightly bound extracellular polymeric substances) into small molecules and disintegration of bioflocs into smaller particles with increased porosity, contact angle, and cell lysis; these changes helped reduce bound water content and improved sludge dewaterability. In addition, the TP-mediated Fenton process disinfected fecal coliforms in the sludge and preserved the sludge organic matters. This work proposes a new paradigm for developing cost-effective sludge dewatering technologies that relies on the synergistic effects of plant polyphenols and advanced oxidation processes.