期刊
ACS APPLIED MATERIALS & INTERFACES
卷 12, 期 23, 页码 25832-25842出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c04169
关键词
atomic dispersion; aerosil; iron-nitrogen-carbon; carbon materials; oxygen reduction reaction
资金
- National Natural Science Foundation of China (NSFC) [NSFC-MAECI 51861135202]
- NSFC of China [NSFC-MAECI 51861135202]
- Ministry of Foreign Affairs and International Cooperation, Italy [NSFC-MAECI 51861135202]
- Fundamental Research Funds for the Central Universities [18CX06063A]
- Royal Society through the Newton Advanced Fellowship award [NAF\R1\191294]
- Newton Fund through the Newton Advanced Fellowship award [NAF\R1\191294]
- LongTerm Subsidy Mechanism from the Ministry of Finance of China
- LongTerm Subsidy Mechanism from the Ministry of Education of China
- Shandong Scientific Research Awards Foundation for Outstanding Young Scientists [ZR2018JL010]
- Program for the Qingdao scientific and technological innovation high-level talents project.aluminum-ion power and energy storage battery [17-2-1-1-zhc]
Utilizing Zn as a fencing agent has enabled the pyrolytic synthesis of atomically dispersed metal-nitrogen-carbon (AD-MNC) materials for broad electrocatalysis such as fuel cells, metal-air batteries, and water electrolyzers. Yet the Zn residue troubles the precise identification of the responsible sites in active service. Herein we developed a simple aerosil-assisted method for preparing AD-MNC materials to cautiously avoid the introduction of Zn. The combined analysis of extended X-ray absorption fine structure (EXAFS) and aberration-corrected high-resolution transition electron microscopy verified the atomic dispersion of Fe species in the as-made Fe-NC sample with a well-defined structure of Fe-N-4. Besides, the EXAFS studies indicated the formation of oxygenated Fe-N-4 moieties (O-Fe-N-4) after the removal of aerosil nanoparticles. Therefore, the immobilization of Fe atoms in the carbon substrate was attributed to the heavily doping N and rich oxygen dangling species at the aerosil surface. Electrochemical measurements revealed that the as-made Fe-NC material furnished with O-Fe-N-4 moieties exhibited excellent oxygen reduction reaction (ORR) performance, characterized by individually indicating similar to 22 mV higher half-wave potentials, with respect to commercial Pt/C catalyst. Density functional theory (DFT) computations suggested that the dangling oxygen ligand on the Fe-N-4 moiety could significantly boost the cleavage of OOH* and the reductive release of *OH intermediates, leading to the enhancement of overall ORR performance.
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