Interface Engineering Enables Robust ZIF-8/N-BaTa 2 O 6 Films for CO 2 Photoreduction via Dynamic CO 2 Enrichment-Activation Synergy

Abstract

The practical application of powder-based photocatalytic CO2 reduction encounters several challenges, including issues related to catalyst recycling, limitations in mass transfer, and inadequate light utilization. This study presents a surfactantguided interfacial engineering method to develop closely integrated ZIF-8/N-doped BaTa2O6 heterostructures, which are further optimized into robust, self-supporting catalytic sheets. The modification of N-doped BaTa2O6 with sodium dodecyl sulfate (SDS) is essential for modulating the nucleation and oriented growth of ZIF-8, resulting in a closely aligned interface that enhances electronic interactions, as evidenced by X-ray photoelectron and Raman spectroscopy analyses. The composite sheet exhibiting the highest performance achieves a CO production rate of 6.5 μmol g -1 h -1 in pure water without requiring sacrificial agents, while retaining the good activity of the powdered form and demonstrating good recyclability. A combination of in situ and post-reaction analyses indicates a dynamic interaction wherein ZIF-8 primarily serves as a CO2 enrichment sponge, while N-doped BaTa2O6 functions as the photoredox catalyst, characterized by an intriguing activation phase. Despite exhibiting a type-I band alignment, the hybrid structure promotes effective charge separation through an interfacial built-in field, which directs electrons toward the concentrated CO2 at the interface for reduction. This research not only highlights a viable pathway for the advancement of photocatalytic devices but also provides critical insights into the dynamic interfacial processes that facilitate CO2 photoreduction.