Efficient simultaneous removal of phosphate and microcystin-LR in water using a novel g-C3N4/calcite composite under dark-visible light cycles

Abstract

Harmful algal blooms (HABs) associated with the abundant presence of phosphorus and microcystin in natural waters have raised a growing global concern. In this study, an adsorption-photocatalysis strategy was developed using a novel g-C3N4/calcite composite for efficient simultaneous removal of phosphate and microcystin-LR in water under dark-visible light cycles for the first time. The appropriate introduction of calcite into g-C3N4 (i.e., g-C3N4/calcite-1) was efficient in both phosphate adsorption (>78.5 %) and microcystin-LR degradation (>84.3 %) under a dark-visible light cycle of 3:3h at an optimal dosage of 100 mg/L in waters (pH 5–9 and temperature 10–40 °C). The simultaneous removal mechanisms proposed that g-C3N4/calcite-1 adsorbed phosphate via adsorption and precipitation with surface Ca2+, and degraded microcystin-LR via oxidation by photogenerated reactive species (mainly h+ and •OH). The material characterizations and density functional theory (DFT) calculations revealed that the combination of g-C3N4 and calcite could not only change the electric field distributions of calcite and optimize the charge transfer during adsorption to improve its adsorption capacity towards phosphate, but also narrow the band gaps of g-C3N4, promote the electron-hole separation and lower the first-step reaction barrier in oxygen reduction pathway during photocatalysis to enhance its visible-light photocatalytic activity towards microcystin-LR. Collectively, these findings are believed to offer valuable insights on the green material design for water environmental remediation and the underlying mechanism elucidation for simultaneous removal of phosphorus and microcystin in water to achieve effective comprehensive management of HABs.