Issue 46, 2023

p-State of surface oxygen for mediating the s-band center of a single-atomic Ag catalyst for enhanced catalytic property for the oxygen reduction reaction

Abstract

The search of excellent electrocatalysts for the two-electron O2-reduction reaction (2e ORR) is of great importance for the green synthesis of H2O2. This study developed a computational framework using density functional theory (DFT) and ab initio molecular dynamic simulation (AIMD) to investigate the influence of acid electrolytes, particularly H coverage, on the s-band center of a single-atomic Ag catalyst, leading to improved catalytic selectivity for the ORR. Specially, the screened catalyst Ag@Ti2C exhibited remarkable intrinsic performance for 2e ORR with an overpotential of only 0.06 V. In acidic electrolytes, Ag@Ti2C selectively bound to O-containing and H species, forming Ag@Ti2CO2Hx. The introduction of O functional groups improved the electron delocalization, enhancing O2–Ag interactions. Significantly, the surface O atom's p-band center exhibited a parabolic trend with the H coverage on Ag@Ti2CO2. Consequently, the catalyst exhibited an optimal overpotential of 0.08 V for 2e ORR at an H atom coverage of 22.2%. It was found that the surface O p-state played a crucial role in mediating the s-band center of the single-atomic Ag catalyst, significantly influencing its catalytic performance in the ORR.

Graphical abstract: p-State of surface oxygen for mediating the s-band center of a single-atomic Ag catalyst for enhanced catalytic property for the oxygen reduction reaction

Supplementary files

Article information

Article type
Paper
Submitted
27 Jul 2023
Accepted
14 Okt 2023
First published
16 Okt 2023

J. Mater. Chem. A, 2023,11, 25399-25409

p-State of surface oxygen for mediating the s-band center of a single-atomic Ag catalyst for enhanced catalytic property for the oxygen reduction reaction

F. Sun, Q. Fang, W. Zhang, C. Lin, W. Chen and G. Zhuang, J. Mater. Chem. A, 2023, 11, 25399 DOI: 10.1039/D3TA04453J

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