Carbon nitride-based Z-scheme heterojunctions for solar-driven advanced oxidation processes

Solar-driven advanced oxidation processes (AOPs) via direct photodegradation or indirect photocatalytic activation of typical oxidants, such as hydrogen peroxide (H₂O₂), peroxymonosulfate (PMS), and peroxydisulfate (PDS), have been deemed to be an efficient technology for wastewater remediation. Artificial Z-scheme structured materials represent a promising class of photocatalysts due to their spatially separated charge carriers and strong redox abilities. Herein, we summarize the development of metal-free graphitic carbon nitride (g-C₃N₄, CN)-based direct and indirect Z-scheme photocatalysts for solar-driven AOPs in removing organic pollutants from water. In the work, the classification of AOPs, definition and validation of Z-schemes are summarized firstly. The innovative engineering strategies (e.g., morphology and dimensionality control, element doping, defect engineering, cocatalyst loading, and tandem Z-scheme construction) over CN-based direct Z-scheme structure are then examined. Rational design of indirect CN-based Z-scheme systems using different charge mediators, such as solid conductive materials and soluble ion pairs, is further discussed. Through examining the relationship between the Z-scheme structure and activity (charge transfer and separation, light absorption, and reaction kinetics), we aim to provide more insights into the construction strategies and structure modification on CN-based Z-schemes towards improving their catalytic performances in AOPs. Lastly, limitations, challenges, and perspectives on future development in this emerging field are proposed.