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 Jūl. 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

To request permission to reproduce material from this article, please go to the Copyright Clearance Center request page.

If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given.

If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page.

Read more about how to correctly acknowledge RSC content.

Social activity

Spotlight

Advertisements