Effective Hole Utilization for Atomically Dispersed Low-Coordination Molybdenum Accelerating Photocatalytic C─H...

Area of Science:

• Materials Science
• Photocatalysis
• Chemical Engineering

Background:

• Acceptorless dehydrogenation of alcohols is a key reaction for producing carbonyl compounds and hydrogen fuel.
• Current photocatalytic methods suffer from inefficient hole utilization due to sluggish alkoxy C-H bond cleavage kinetics.

Purpose of the Study:

• To develop a novel photocatalyst for enhanced acceptorless dehydrogenation of alcohols.
• To improve the efficiency of C-H bond activation and the utilization of photogenerated holes.

Main Methods:

• Synthesis of ultrathin ZnIn2S4 nanosheets decorated with atomically dispersed low-coordination molybdenum.
• Photocatalytic experiments using benzyl alcohol as a model substrate.
• Extensive characterization including experimental and theoretical calculations.

Main Results:

• Achieved an internal quantum efficiency of 45.2% at 400 nm.
• Obtained 99% selectivity for benzaldehyde production from benzyl alcohol.
• Demonstrated that low-coordination Mo traps holes efficiently, enhancing their lifetime and diffusion.

Conclusions:

• Atomically dispersed low-coordination Mo on ultrathin ZnIn2S4 significantly accelerates photocatalytic C-H activation.
• The enhanced performance is attributed to improved hole trapping, extended lifetime, and optimized C-H activation driving force.
• This work represents a significant advancement in improving hole utilization for photocatalysis.