Integration of Single-Atom Catalyst with Z-Scheme Heterojunction for Cascade Charge Transfer Enabling Highly Efficient Piezo-Photocatalysis.

Piezo-assisted photocatalysis (namely, piezo-photocatalysis), which utilizes mechanical energy to modulate spatial and energy distribution of photogenerated charge carriers, presents a promising strategy for molecule activation and reactive oxygen species (ROS) generation toward applications such as environmental remediation. However, similarly to photocatalysis, piezo-photocatalysis also suffers from inferior charge separation and utilization efficiency. Herein, a Z-scheme heterojunction composed of single Ag atoms-anchored polymeric carbon nitride (Ag-PCN) and SnO 2- x is developed for efficient charge carrier transfer/separation both within the catalyst and between the catalyst and surface oxygen molecules (O 2 ). As revealed by charge dynamics analysis and theoretical simulations, the synergy between the single Ag atoms and the Z-scheme heterojunction initiates a cascade electron transfer from SnO 2- x to Ag-PCN and then to O 2 adsorbed on Ag. With ultrasound irradiation, the polarization field generated within the piezoelectric hybrid further accelerates charge transfer and regulates the O 2 activation pathway. As a result, the Ag-PCN/SnO 2- x catalyst efficiently activates O 2 into ·O 2 - , ·OH, and H 2 O 2 under co-excitation of visible light and ultrasound, which are consequently utilized to trigger aerobic degradation of refractory antibiotic pollutants. This work provides a promising strategy to maneuver charge transfer dynamics for efficient piezo-photocatalysis by integrating single-atom catalysts (SACs) with Z-scheme heterojunction.

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