A pyrolysis-free path toward superiorly catalytic nitrogen-coordinated single atom

Area of Science:

• Electrochemistry
• Materials Science
• Catalysis

Background:

• Nitrogen-coordinated single-atom catalysts (SACs) offer high atom utilization and activity for electrocatalysis.
• Current synthesis methods often involve high-temperature pyrolysis, leading to structural instability and random atom distribution.
• Developing precise and operable synthesis strategies for SACs is crucial for practical applications.

Purpose of the Study:

• To develop a pyrolysis-free synthetic approach for preparing highly active SACs.
• To utilize a π-conjugated iron phthalocyanine (FePc)-rich covalent organic framework (COF) for catalyst synthesis.
• To investigate the electrocatalytic performance of the synthesized SACs in oxygen reduction and zinc-air batteries.

Main Methods:

• Synthesized SACs using a fully π-conjugated iron phthalocyanine (FePc)-rich covalent organic framework (COF).
• Employed a pyrolysis-free strategy to anchor atomically well-designed Fe-N-C centers via intermolecular interactions between COF and graphene.
• Evaluated catalyst performance in oxygen reduction reactions and zinc-air batteries.

Main Results:

• The synthesized SACs exhibited exceptional kinetic current density for oxygen reduction, four times higher than benchmark Pt/C.
• Demonstrated superior power density and cycling stability in zinc-air batteries compared to Pt/C.
• The pyrolysis-free method ensured precise anchoring of Fe-N-C centers, avoiding random atom distribution.

Conclusions:

• The developed pyrolysis-free method enables the synthesis of highly active and stable SACs.
• FePc-rich COF-based SACs represent a promising alternative to traditional platinum catalysts for oxygen reduction and energy storage applications.
• This approach offers a pathway for controllable synthesis of advanced single-atom catalysts.