Issue 11, 2021

Theoretical insight into single Rh atoms anchored on N-doped γ-graphyne as an excellent bifunctional electrocatalyst for the OER and ORR: electronic regulation of graphitic nitrogen

Abstract

Reducing the overpotential and increasing the reaction rate, which are respectively determined by the thermodynamics and kinetics of electrocatalysis, are the keys to obtaining high-performance bifunctional electrocatalysts for the OER/ORR. Herein, six late-transition metals (Ru, Rh, Pd, Os, Ir, and Pt) anchored on γ-GY and graphitic N doped γ-GY substrates are screened as electrocatalysts for the OER and ORR via density functional theory, and the effects of electronic regulation due to the presence of graphitic N on the thermodynamics and kinetics of electrocatalysis are investigated in detail. Among the six γ-GY@TM candidates, only γ-GY@Rh exhibits excellent OER activity, with an overpotential of 0.42 V. Furthermore, graphitic N doped graN-γ-GY@Rh shows outstanding bifunctional electrocatalytic activity, with overpotentials of 0.27 V for the OER and 0.33 V for the ORR, which are remarkably superior to the values of 0.43 V for RuO2 and 0.45 V for noble-metal Pt electrocatalysts. The present results present some of the lowest overpotentials for OER/ORR electrocatalysts given by theoretical studies to date. From a kinetics point of view, N-doping also remarkably reduces the activation energy barriers of the catalytic rate-limiting steps of the OER and ORR, accelerating the reaction processes and significantly improving the conductivity. Our work provides a theoretical strategy for designing high-efficiency bifunctional OER/ORR electrocatalysts based on γ-GY materials.

Graphical abstract: Theoretical insight into single Rh atoms anchored on N-doped γ-graphyne as an excellent bifunctional electrocatalyst for the OER and ORR: electronic regulation of graphitic nitrogen

Supplementary files

Article information

Article type
Paper
Submitted
20 Oct 2020
Accepted
26 Feb 2021
First published
27 Feb 2021

Nanoscale, 2021,13, 5800-5808

Theoretical insight into single Rh atoms anchored on N-doped γ-graphyne as an excellent bifunctional electrocatalyst for the OER and ORR: electronic regulation of graphitic nitrogen

Y. Qin, M. Yang, C. Deng, W. Shen, R. He and M. Li, Nanoscale, 2021, 13, 5800 DOI: 10.1039/D0NR07513B

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