Creating Asymmetric Fe-NC-N Sites in Single-Atom Catalysts Boosts Catalytic Performance for Oxygen Reduction Reaction.

Fine tuning of the metal site coordination environment of a single-atom catalyst (SAC) to boost its catalytic activity for oxygen reduction reaction (ORR) is of significance but challenging. Herein, we report a new SAC bearing Fe-NC-N sites with asymmetric in-plane coordinated Fe-NC and axial coordinated N atom for ORR, which was obtained by pyrolysis of an iron isoporphyrin on polyvinylimidazole (PVI) coated carbon black. The C@PVI-(NCTPP)Fe-800 catalyst exhibited significantly improved ORR activity ( = 0.

Contracted Fe-N-C Sites in Single-Atom Catalysts Boosting Catalytic Performance for Oxygen Reduction Reaction.

Promoting the catalyst performance for oxygen reduction reaction (ORR) in energy conversion devices through controlled manipulation of the structure of catalytic active sites has been a major challenge. In this work, we prepared Fe-N-C single-atom catalysts (SACs) with Fe-N active sites and found that the catalytic activity of the catalyst with shrinkable Fe-N-C sites for ORR was significantly improved compared with the catalyst bearing normal Fe-N-C sites. The catalyst C@PVI-(TPC)Fe-800, prepared by pyrolyzing an axial-imidazole-coordinated iron corrole precursor, exhibited positive shifted half-wave potential ( = 0.

Design and Preparation of Fe-N Catalytic Sites in Single-Atom Catalysts for Enhancing the Oxygen Reduction Reaction in Fuel Cells.

There is an urgent need for developing nonprecious metal catalysts to replace Pt-based electrocatalysts for oxygen reduction reaction (ORR) in fuel cells. Atomically dispersed M-N/C catalysts have shown promising ORR activity; however, enhancing their performance through modulating their active site structure is still a challenge. In this study, a simple approach was proposed for preparing atomically dispersed iron catalysts embedded in nitrogen- and fluorine-doped porous carbon materials with five-coordinated Fe-N sites.

Bioinspired Transition-Metal Complexes as Electrocatalysts for the Oxygen Reduction Reaction.

The oxygen reduction reaction (ORR) is one of the most important reactions in life processes and energy conversion systems. To alleviate global warming and the energy crisis, the development of high-performance electrocatalysts for the ORR for application in energy conversion and storage devices such as metal-air batteries and fuel cells is highly desirable. Inspired by the biological oxygen activation/reduction process associated with heme- and multicopper-containing metalloenzymes, iron and copper-based transition-metal complexes have been extensively explored as ORR electrocatalysts.

Efficient electrocatalytic O reduction at copper complexes grafted onto polyvinylimidazole coated carbon nanotubes.

A facile approach to prepare Cu complexes for an efficient oxygen reduction reaction (ORR) was developed. Copper complexes of 5-nitrophenanthroline were sandwiched between polyvinylimidazole layers wrapped on carbon nanotubes, which showed ORR activity comparable to a Pt/C catalyst in alkaline media.