Sequential element control of non-precious dual atom catalysts on mesoporous carbon nanotubes for high performance lithium-oxygen batteries

• Published in: Journal of materials chemistry. A, Materials for energy and sustainability Vol. 12; no. 42; pp. 28953 - 28964
• Main Authors: Lim, Yeji, Chang, Hongjun, Kim, Huiju, Yoo, Yoon Jeong, Rho, YeoJin, Kim, Bo Ran, Byon, Hye Ryung, Moon, Janghyuk, Ryu, Won-Hee
• Format: Journal Article
• Language: English
• Published: Cambridge Royal Society of Chemistry 29.10.2024
• Subjects: Carbon; Carbon nanotubes; Catalysis; Catalysts; Catalytic activity; Density functional theory; Energy storage; Heavy metals; Iron; Life span; Lithium; Nanotechnology; Nanotubes; Nickel; Nitrogen dioxide; Noble metals; Oxygen; Reaction mechanisms
• ISSN: 2050-7488; 2050-7496
• DOI: 10.1039/d4ta05490c

Lithium-oxygen (Li-O 2 ) batteries, recognized as candidates for the highest energy storage, face challenges of irreversibility and low efficiency due to insulating discharge products. Addressing these issues, our study explores innovative dual-atom catalysts (DACs) comprising non-precious metals, specifically atomically scaled nickel (Ni) and iron (Fe), positioned on defective mesopore sites of nitrogen-doped carbon nanotubes (NCNTs) to enhance battery performance. We successfully achieved the synthesis of both homogeneous (Fe-Fe-NCNTs and Ni-Ni-NCNTs) and heterogeneous (Ni-Fe-NCNTs and Fe-Ni-NCNTs) DACs on NCNTs, by varying the loading sequences and combination of Ni and Fe. Our findings demonstrate that Fe-first-loaded DACs, particularly heterogeneous Ni-Fe-NCNT variants, excelled in both NO 2 − mediation reactivity and catalytic activity, achieving a longer lifespan of 200 cycles and maintaining consistent ORR/OER overpotential. Insights into the mesoporous loading sites and reaction mechanisms of these DACs in Li-O 2 cells were gained through density functional theory calculations. This research paves the way for replacing costly noble metal catalysts with tailored non-noble metal combinations, potentially revolutionizing Li-O 2 cell technology and broadening applications in heterogeneous catalysis. Introducing nickel and iron based homogeneous and heterogeneous dual atom catalysts (DACs) onto N-doped carbon nanotube defect sites significantly enhances Li-O 2 cell performance.