Abstract
While there is much potential for photocatalytic CO2 reduction, poor light absorption and high recombination rates of photogenerated charges limit its effectiveness. To address these challenges, we systematically developed a heterointerface-engineered ternary hybrid photocatalyst comprising NiAl-layered double hydroxide (LDH), titanium dioxide (TiO2), and titanium carbide (Ti3C2) MXene via an in situ growth approach. As a result of the unique combination of these three components, the synthesized ternary NiAl-LDH@TiO2/Ti3C2 photocatalyst demonstrated broad light absorption spanning across the ultraviolet, visible, and near-infrared regions, as well as elevated CO2 adsorption capacity. In situ-irradiated X-ray photoelectron spectroscopy and electron paramagnetic resonance analyses provided compelling evidence for an unconventional S-scheme charge transfer mechanism in the ternary system that effectively separates the charges and suppresses recombination, allowing NiAl-LDH to maintain its strong reducing capacity and TiO2 to maintain its robust oxidizing capacity. Utilizing the complementary and synergistic properties of these three components (NiAl-LDH, TiO2, and Ti3C2), an optimized ternary NiAl-LDH@TiO2/Ti3C2 photocatalyst with 30 wt% Ti3C2 exhibited extraordinary solar-driven CO2 reduction performance with a remarkable 99 % CO selectivity against competitive H2 production and a high apparent quantum yield of 0.81 at 365 nm. Additionally, the ternary photocatalyst exhibited excellent stability, maintaining its performance capacity over multiple CO2 reduction cycles. This work provides a fresh perspective on designing and creating efficient ternary S-scheme photocatalytic systems for solar-driven CO2 reduction and highlights the potential for energy-rich fuel production.
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