Multi-field coupling enhanced plasmonic Mo^δ+ active site to efficiently hydrolyze ammonia borane.

Area of Science:

• Materials Science
• Catalysis
• Renewable Energy

Background:

• Solar-driven ammonia borane hydrolysis is crucial for hydrogen production but hindered by carrier recombination and inefficient hot electron injection.
• Developing efficient catalysts is key to overcoming these limitations for practical applications.

Purpose of the Study:

• To enhance solar-driven ammonia borane hydrolysis activity using plasmon polarization-induced multi-field coupling.
• To investigate the role of reconstructed surface unsaturated Mo active sites in catalysis.
• To leverage machine learning for catalyst design and optimization.

Main Methods:

• Utilized machine learning to guide the development of plasmon polarization-induced multi-field coupling.
• Synthesized and characterized reconstructed surface unsaturated Mo active sites.
• Investigated catalytic performance and stability in ammonia borane hydrolysis over 100 hours.
• Analyzed carrier separation, electron accumulation, and hot electron delocalization mechanisms using electric field effects.

Main Results:

• Achieved a high turnover frequency of 5806 min⁻¹ for ammonia borane hydrolysis, surpassing many reported catalysts.
• Demonstrated excellent catalytic activity and stability (>100 hours) with reconstructed surface unsaturated Mo active sites.
• Verified that polarized electric fields enhance carrier separation and electron accumulation.
• Showcased efficient hot electron delocalization and channeling via plasmon oscillation, lowering reaction barriers.

Conclusions:

• Plasmon polarization-induced multi-field coupling effectively enhances solar-driven ammonia borane hydrolysis.
• Unsaturated Mo active sites exhibit superior activity and stability, driven by facilitated carrier dynamics and efficient hot electron transfer.
• This approach offers a competitive and stable catalytic system for hydrogen generation from ammonia borane.