Solar-Driven Carbon-Nitrogen Coupling Between Biomass-Derived Alcohol and Ammonia for High-Value Amine Synthesis

Area of Science:

• Catalysis
• Materials Science
• Green Chemistry

Background:

• Biomass-derived alcohols offer a sustainable feedstock for chemical synthesis.
• Photocatalytic carbon-nitrogen (C-N) coupling is a promising route to amines but faces challenges in C-H activation and nitrogen conversion.
• Existing catalysts often suffer from low efficiency and selectivity in amine synthesis.

Purpose of the Study:

• To develop an efficient photocatalyst for C-N coupling of biomass-derived alcohols and ammonia.
• To elucidate the synergistic redox pathway enabling enhanced catalytic activity.
• To demonstrate the catalyst's applicability in scalable, solar-driven amine production.

Main Methods:

• Synthesis of atomically dispersed Au species coordinated with phosphorus on CdS nanorods (AuP3-CdS).
• In situ spectroscopy and theoretical calculations to investigate reaction mechanisms.
• Photocatalytic experiments using biomass-derived furfuryl alcohol and ammonia.
• Evaluation of catalyst performance under concentrated natural sunlight.

Main Results:

• AuP3-CdS exhibits a synergistic redox pathway, enhancing both alcohol dehydrogenation and imine hydrogenation.
• Achieved a furfurylamine production rate of 41.48 mmol g⁻¹ h⁻¹ with 99.1% selectivity, 63 times higher than AuS3-CdS.
• Demonstrated broad applicability for various alcohols and successful solar-driven synthesis in a scalable reactor (14.24 mmol g⁻¹ h⁻¹, 97.1% selectivity).

Conclusions:

• The AuP3-CdS catalyst, with its unique Au-P3 active sites, significantly advances photocatalytic amine synthesis.
• This work presents a viable and scalable strategy for producing valuable amines from renewable biomass resources using solar energy.