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Inhibitory effects of phosphate on zero-valent iron (ZVI) dissolution have been studied mainly focusing on a single chemical system. Little is known about inhibitory effects and the mechanism of phosphate on ZVI dissolution within a bioreactor during long-term operation. This study demonstrates the feasibility of achieving energy recovery from phosphate-containing domestic sewage using an efficient anaerobic reactor with micro-sized or nano-sized ZVI addition. The results indicate that the chemical oxygen demand (COD) removal and methane production are enhanced by ZVI addition. A maximum COD removal efficiency of 89% and methane content of 60% was achieved. However, the strengthening effect of ZVI on methane production is weakened by the presence of phosphate in domestic sewage. Analyzing the variations of Fe2+ ions and phosphate concentrations and characterizing the micro-morphology of corroded ZVI proved that the generated Fe2+ ions reacts with phosphate and forms a passivation layer on the ZVI surface, inhibiting further dissolution of ZVI. As an improved alternative, we chose the double layered core-shell structured ZVI@carbon composite as an excellent candidate to reduce the inhibitory effects of phosphate on ZVI dissolution. In this way, the direct formation of precipitates on the ZVI surface can be avoided due to the protective carbon layer which adjusts the ion transfer. Adding ZVI@carbon composites accelerate the methane content by 16%. To our knowledge, this is the first report on adding ZVI@carbon composites to promote the anaerobic metabolism in studies, which are focusing on reducing the inhibition of ZVI by phosphate.