Deep Electronic State Regulation through Unidirectional Cascade Electron Transfer Induced by Dual Junction Boosting...

Area of Science:

• Materials Science
• Electrochemistry
• Catalysis

Background:

• Unidirectional cascade electron transfer is crucial for regulating catalytic active sites but is underexplored in electrocatalysis.
• Designing advanced heterostructures is key to improving catalytic efficiency for reactions like oxygen reduction.

Purpose of the Study:

• To design and investigate a dual-junction heterostructure for enhanced electrocatalysis.
• To explore the mechanism of unidirectional cascade electron transfer for oxygen reduction reaction (ORR) activity.

Main Methods:

• Fabrication of a dual junction heterostructure: iron phthalocyanine (FePc)/MXene (L-Ti3C2-R) anchored on g-C3N4 nanosheets.
• Investigation of unidirectional cascade electron transfer pathways (g-C3N4 → L-Ti3C2-R → FePc).
• Electrochemical characterization of the oxygen reduction reaction (ORR) activity of the synthesized catalyst.

Main Results:

• The FePc/L-OH/CN catalyst exhibited a high half-wave potential (E1/2) of 0.92 V for ORR, outperforming Pt/C (0.85 V).
• Unidirectional cascade electron transfer facilitated by the dual junction enriched the Fe center, enhancing O2 adsorption.
• Axial Fe-O coordination in alkalized MXene (L-Ti3C2-OH) further improved electron transfer between FePc and MXene.

Conclusions:

• The developed dual-junction heterostructure effectively regulates electronic states via unidirectional cascade electron transfer, boosting ORR performance.
• This strategy offers a new approach for designing efficient electrocatalysts by controlling multi-step charge transfer.
• The findings can be extended to other proton-coupled electron transfer processes, advancing catalyst design.