» Articles » PMID: 29891686

Unveiling the High-activity Origin of Single-atom Iron Catalysts for Oxygen Reduction Reaction

Overview
Specialty Science
Date 2018 Jun 13
PMID 29891686
Citations 31
Authors
Affiliations
Soon will be listed here.
Abstract

It is still a grand challenge to develop a highly efficient nonprecious-metal electrocatalyst to replace the Pt-based catalysts for oxygen reduction reaction (ORR). Here, we propose a surfactant-assisted method to synthesize single-atom iron catalysts (SA-Fe/NG). The half-wave potential of SA-Fe/NG is only 30 mV less than 20% Pt/C in acidic medium, while it is 30 mV superior to 20% Pt/C in alkaline medium. Moreover, SA-Fe/NG shows extremely high stability with only 12 mV and 15 mV negative shifts after 5,000 cycles in acidic and alkaline media, respectively. Impressively, the SA-Fe/NG-based acidic proton exchange membrane fuel cell (PEMFC) exhibits a high power density of 823 mW cm Combining experimental results and density-functional theory (DFT) calculations, we further reveal that the origin of high-ORR activity of SA-Fe/NG is from the Fe-pyrrolic-N species, because such molecular incorporation is the key, leading to the active site increase in an order of magnitude which successfully clarifies the bottleneck puzzle of why a small amount of iron in the SA-Fe catalysts can exhibit extremely superior ORR activity.

Citing Articles

Why Do Weak-Binding M-N-C Single-Atom Catalysts Possess Anomalously High Oxygen Reduction Activity?.

Zhang D, She F, Chen J, Wei L, Li H J Am Chem Soc. 2025; 147(7):6076-6086.

PMID: 39924878 PMC: 11848820. DOI: 10.1021/jacs.4c16733.


Molecular Strain Accelerates Electron Transfer for Enhanced Oxygen Reduction.

Musgrave 3rd C, Su J, Xiong P, Song Y, Huang L, Liu Y J Am Chem Soc. 2025; 147(4):3786-3795.

PMID: 39818842 PMC: 11783534. DOI: 10.1021/jacs.4c16637.


Advancements on Single-Atom Catalysts-Mediated Persulfate Activation: Generating Reactive Species for Contaminants Elimination in Water.

Yu W, Xu Y Molecules. 2024; 29(23).

PMID: 39683855 PMC: 11643893. DOI: 10.3390/molecules29235696.


Benchmarking a Molecular Flake Model on the Road to Programmable Graphene-Based Single-Atom Catalysts.

Gallagher C, Siddiqui W, Arnold T, Cheng C, Su E, Zhao Q J Phys Chem C Nanomater Interfaces. 2024; 128(7):2876-2883.

PMID: 38414836 PMC: 10895666. DOI: 10.1021/acs.jpcc.3c07681.


Real-time tracking of electron transfer at catalytically active interfaces in lithium-ion batteries.

Li H, Hu Z, Zuo F, Li Y, Liu M, Liu H Proc Natl Acad Sci U S A. 2024; 121(7):e2320030121.

PMID: 38315861 PMC: 10873553. DOI: 10.1073/pnas.2320030121.


References
1.
Chung H, Cullen D, Higgins D, Sneed B, Holby E, More K . Direct atomic-level insight into the active sites of a high-performance PGM-free ORR catalyst. Science. 2017; 357(6350):479-484. DOI: 10.1126/science.aan2255. View

2.
Sa Y, Seo D, Woo J, Lim J, Cheon J, Yang S . A General Approach to Preferential Formation of Active Fe-N Sites in Fe-N/C Electrocatalysts for Efficient Oxygen Reduction Reaction. J Am Chem Soc. 2016; 138(45):15046-15056. DOI: 10.1021/jacs.6b09470. View

3.
Jiao Y, Zheng Y, Jaroniec M, Qiao S . Design of electrocatalysts for oxygen- and hydrogen-involving energy conversion reactions. Chem Soc Rev. 2015; 44(8):2060-86. DOI: 10.1039/c4cs00470a. View

4.
Yin P, Yao T, Wu Y, Zheng L, Lin Y, Liu W . Single Cobalt Atoms with Precise N-Coordination as Superior Oxygen Reduction Reaction Catalysts. Angew Chem Int Ed Engl. 2016; 55(36):10800-5. DOI: 10.1002/anie.201604802. View

5.
Zhang H, Hwang S, Wang M, Feng Z, Karakalos S, Luo L . Single Atomic Iron Catalysts for Oxygen Reduction in Acidic Media: Particle Size Control and Thermal Activation. J Am Chem Soc. 2017; 139(40):14143-14149. DOI: 10.1021/jacs.7b06514. View