Precious trimetallic single-cluster catalysts for oxygen and hydrogen electrocatalytic reactions: Theoretical considerations

• Published in: Nano research Vol. 16; no. 5; pp. 8042 - 8050
• Main Authors: Shi, Xiaochuan, Li, Yongcheng, Zhang, Shan, Hu, Riming, Gao, Shuang, Jin, Peipeng, Shang, Jiaxiang, Shui, Jianglan
• Format: Journal Article
• Language: English
• Published: Beijing Tsinghua University Press 01-05-2023; Springer Nature B.V
• Subjects: Alloys; Atomic/Molecular Structure and Spectra; Biomedicine; Biotechnology; Carbon; Catalysis; Catalysts; Catalytic oxidation; Chemical reduction; Chemistry and Materials Science; Clusters; Condensed Matter Physics; Density functional theory; Electrocatalysts; Electronic structure; Energy; Free energy; Heat of formation; Hybridization; Hydrogen; Hydrogen evolution reactions; Iridium; Materials Science; Mathematical analysis; Metals; Nanotechnology; Noble metals; Oxygen; Oxygen evolution reactions; Oxygen reduction reactions; Palladium; Platinum; Precious metals; Research Article; Single atom catalysts; oxygen evolution reaction; trimetallic catalysts; oxygen reduction reaction; single-cluster catalysts; density functional theory
• ISSN: 1998-0124; 1998-0000
• DOI: 10.1007/s12274-022-5347-6

Single cluster catalysts (SCCs), which exhibit remarkable catalytic performance due to their high metal loading and synergy effect between metal atoms, have attracted great attention in research. Herein, by means of density functional theory calculations, the oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and hydrogen evolution reaction (HER) performances of precious metal (Pt, Pd, Rh, and Ir) trimetallic single-cluster electrocatalyst (U
x
V
y
W
z
-NG) are investigated. The calculation results show that Pt, Pd, and Ir have significant effect on ORR, OER, and HER, respectively, and all the calculated U
x
V
y
W
z
-NG structures are thermodynamically stable due to the negative formation energies and binding energies. The Pt
3
-NG, Pd
3
-NG, and Ir
3
-NG show the lowest ORR, OER, and HER overpotentials of 0.63, 0.77, and −0.02 V, respectively, among all combinations of U
x
V
y
W
z
-NG. These overpotentials are lower than that of precious metal single atom catalysts (SACs), which indicate better activities of precious trimetallic SCCs than those of SACs. The electronic structure reveals that the O-2p orbital shows strong hybridization strength with Pt-3d orbitals in the system of OH adsorbed Pt
3
-NG and thus facilitates the electrocatalytic reactions. The results are helpful for the rational design of high-performance triatomic catalysts.