摘要
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•APP surface engineering enabled precise interfacial modification of Al-doped ZnO nanosheet arrays.•Plasma-induced oxygen vacancies strategically narrowed the bandgap, enhancing light harvesting.•Engineered surface states reduced charge-transfer resistance and suppressed carrier recombination.•Enhanced bifunctional activity for solar-driven hydrogen evolution and pollutant mineralization.•Monolithic growth on Al foil provides binder-free stability and robust recovery-free recyclability.
The rational architecture of bifunctional photocatalytic systems represents a paramount frontier for energy conversion and environmental remediation. This work elucidates a sustainable, high-throughput surface-modification protocol utilizing atmospheric pressure plasma (APP) to construct a high-performance, bifunctional photocatalytic system. The engineered Al-doped ZnO nanosheet architectures achieve simultaneous renewable energy production and photocatalytic dye degradation by promoting the utilization of photogenerated electron-hole pairs, thereby addressing the distinct goals of solar-to-fuel conversion and environmental remediation through an integrated interfacial charge-transfer mechanism. The implementation of a finely tuned APP process (50 W for 60 s) effectively modified the surface defect environment, as supported by the increased oxygen-vacancy-related contribution observed in the O 1s XPS analysis of the optimized sample. Consequently, the optimized sample exhibited a competitive co-catalyst-free H2 production performance, achieving up to 358.8 ± 45.3 μmol·h−1·g−1 under simulated solar flux. Furthermore, the plasma-engineered surface states promoted rapid interfacial charge-transfer kinetics, leading to an approximately two-fold enhancement in the apparent degradation kinetics of methyl orange compared to unmodified specimens. The immobilized nanosheet configuration further provided exceptional photostability and robust recyclability over five consecutive cycles, underscoring the potential of APP-assisted surface engineering for the scalable fabrication of multifunctional metal-oxide photocatalysts.