Interfacial Modification of Conjugated Coordination Polymers for Efficient and Selective Nitrogen Electroreduction to...

Area of Science:

• Materials Science
• Electrochemistry
• Catalysis

Background:

• Electrocatalytic nitrogen reduction reaction (NRR) to ammonia offers sustainable synthesis at ambient conditions.
• Single-atom catalysts show promise for NRR due to high metal utilization and unique active sites.
• Challenges remain in controlling coordination structures and reaction microenvironments for improved NRR selectivity and activity.

Purpose of the Study:

• To develop a facile and general strategy for preparing a composite catalyst for enhanced NRR.
• To investigate the effect of protic ionic liquids (PIL) modification on single-atom catalysts within conjugated coordination polymers.
• To improve both the selectivity and activity of the electrocatalytic nitrogen reduction reaction.

Main Methods:

• Synthesis of a composite catalyst by modifying conjugated coordination polymers with protic ionic liquids (PIL).
• Characterization of the catalyst's structure and properties.
• Electrocatalytic performance testing for the nitrogen reduction reaction (NRR) and theoretical calculations to understand reaction mechanisms.

Main Results:

• The PIL-modified composite catalyst significantly outperformed the unmodified counterpart.
• Profound electronic interactions between PIL and conjugated coordination polymers were observed.
• PIL modification decreased the thermodynamic energy barrier for NRR and created a favorable microenvironment, enhancing NRR selectivity and activity.

Conclusions:

• A novel interfacial modification strategy using PIL on conjugated coordination polymers is effective for designing high-performance single-atom catalysts.
• This approach provides a viable method for low-cost, efficient ammonia synthesis via electrocatalytic NRR.
• The findings offer a pathway for developing advanced catalysts for energy conversion applications.