Stabilization of lanthanide single-atom active sites via interlayer confinement and coordination anchoring toward high-performance photocatalytic hydrogen evolution

Photocatalytic water splitting offers a sustainable pathway for hydrogen production. Lanthanide (Ln), with unique 4f electron configurations and strong spin-orbit coupling, exhibits superior catalytic properties. However, their practical deployment is hindered by severe aggregation due to weak meta-ligand interactions and thermodynamic instability. Herein, we report a dual-stabilization strategy combining interlayer confinement and robust Ln–O coordination within a coordination-driven self-assembly framework. This approach enables uniform dispersion of Ln atoms in layered self-assembled carbon nitride (S-CN), effectively suppressing aggregation and enhancing atomic stability. The Sm@S-CN catalyst exhibits an eightfold enhancement in hydrogen evolution activity relative to its undoped counterparts and demonstrates remarkable stability over a duration of 100 h. Additional π - π stacking with conjugated porphyrin molecules broadens light absorption and facilitates charge transfer, achieving a high hydrogen evolution rate of 200.5 mmol g −1 h −1 . This scalable strategy provides a universal platform for stabilizing the Ln single-atom charge modulation center and offers promising prospects for solar-driven hydrogen production.