Tandem photocatalysis of nitrate to nitrogen on Cu@CN/TiOx S-scheme heterojunction

Abstract

The persistent challenge of nitrate (NO3–) pollution in water systems, profoundly impacting ecosystems and human health, demands effective remediation strategies. Here, we present an innovative S-scheme Cu@CN/TiOx heterojunction for high-efficiency photocatalytic denitrification (PCDN). Evaluation of its performance demonstrates exceptional NO3– removal efficiency (99.5%) and remarkable N2 selectivity (95.5%), with 13.7 and 4.1 times higher rate constants of NO3– removal than the individual Cu@CN and TiOx components. Notably, this catalyst exhibits impressive stability across multiple cycles, maintaining consistent high conversion rates and selectivity. Mechanistic insights unveiled a tandem reaction pathway where Cu@CN selectively reduced NO3– to NO2–, followed by the TiOx-mediated CO2•– generation, enabling highly selective NO2– to N2 conversion. This unique catalytic system, featuring spatially separated redox-active sites, presents a promising avenue for efficient, selective, and stable denitrification processes, offering significant potential in addressing water pollution challenges and advancing tandem catalytic systems.