Reconstruction-hybridization of molecular and metallic interfaces for efficient oxygen evolution

Area of Science:

• Electrochemistry
• Materials Science
• Catalysis

Background:

• Electrochemical reconstruction of molecular catalysts is key for high-performance oxygen evolution reaction (OER) interfaces.
• The specific roles of the molecular center and substrate in this process are not fully understood.

Purpose of the Study:

• To investigate the roles of molecular precursors and catalytic hosts in electrochemical reconstruction for OER.
• To establish design principles for efficient multi-metal OER catalysts.

Main Methods:

• Utilized a "reconstruction-hybridization" strategy with metal phthalocyanines (M1Pc) as precursors and metal foils (M2) as hosts.
• Employed in situ and ex situ characterization techniques.
• Systematically screened various metal combinations (Fe, Co, Ni, Cu) for M1 and M2.

Main Results:

• FePc/Ni system transformed Fe-N4 sites into a disordered, oxygen-coordinated Fe-containing interface on the Ni substrate.
• This interface enhances OER by accelerating intermediate adsorption and charge transfer.
• Established that M1 (precursor) modulates interfacial reconstruction, while M2 (host) acts as the active catalyst.

Conclusions:

• Demonstrated non-interchangeable roles for M1 (modulator) and M2 (active host) in electrochemical reconstruction.
• Provided mechanistic insights into dynamic interface formation.
• Offered a framework for designing efficient multi-metal OER catalysts via electrochemical reconstruction.