Due to the highly reductive capacity of nano zero-valent iron (nZVI), the reduction of nitrate (NO3--N) is prone to produce ammonia (NH4+-N) as a by-product and has low selectivity for nitrogen gas (N2). Selective conversion of NO3--N to harmless N2 by regulating reaction pathway is the key to improve the reduction and nitrogen removal performance of nZVI-based materials. In this study, metal copper (Cu) was added to nZVI to prepare Cu-nZVI/LDH bimetallic composites. Cu was used as a catalyst to form a galvanic coupling with nZVI to accelerate electron transfer and improve the electron utilization efficiency. Synergism of adsorption and reduction of NO3--N was achieved through adsorption of layered bimetallic hydroxide (LDH) and reduction of nZVI. The results showed that the NO3--N removal and N2 product selectivity by Cu-nZVI/LDH was as high as 95.6% and 80.3%, respectively. The critical reaction pathway of N2 generation on the Cu surface of Cu-nZVI/LDH composite was further revealed by DFT theoretical calculations. Experiments on actual micro-polluted water showed that the removal of NO3--N by Cu-nZVI/LDH reached 85.2%. The NO3--N removal of the composite material slightly decreased to 78.6% after 15 d of aging, verifying that the composite material had good potential for practical applications.
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