Boosting activity toward oxygen reduction reaction of a mesoporous FeCuNC catalyst via heteroatom doping-induced electronic state modulation

• Published in: Journal of materials chemistry. A, Materials for energy and sustainability Vol. 10; no. 10; pp. 5361 - 5372
• Main Authors: Kim, Jong Gyeong, Cho, Jinwon, Han, Sunghoon, Lee, Hyejin, Yuk, Eunsung, Bae, Byungchan, Jang, Seung Soon, Pak, Chanho
• Format: Journal Article
• Language: English
• Published: Cambridge Royal Society of Chemistry 08.03.2022
• Subjects: Alternative fuels; Catalysts; Chemical reduction; Copper; Density functional theory; Doping; Electron states; Fuel cells; Fuel technology; Oxygen; Oxygen reduction reactions
• ISSN: 2050-7488; 2050-7496
• DOI: 10.1039/D1TA07264A

Non-precious metal catalysts for oxygen reduction reaction (ORR) are promising alternatives to Pt/C in fuel cells, thus, demand for advanced catalysts is arising. Herein, we prepared and characterized mesoporous Fe and Cu anchored in N-, S-, and P-doped carbon (FeCu x NC) catalysts, revealing the presence of ordered mesoporous grain-shaped particles and demonstrating that the electronic state of the active sites (Fe–N x ) is controlled by their environments, which can affect ORR kinetics. Half-cell measurements revealed that FeCu x NC promoted ORRs more effectively (0.92 V at 3 mA cm −2 ) than Pt/C (0.87 V at 3 mA cm −2 ) in alkaline conditions, while a current density of 490 mA cm −2 was achieved at 0.6 V in a single-cell level. Multi-heteroatom doping modulated the energy of OOH* and OH − adsorption on the active sites, and the lowest overpotential (according to density functional theory calculations) was obtained for the Fe–Cu–N 3 –C–P–S model.