Issue 10, 2024

Ni clusters immobilized on oxygen-rich siloxene nanosheets for efficient electrocatalytic oxygen reduction toward H2O2 synthesis

Abstract

Hydrogen peroxide (H2O2) electrosynthesis via the two-electron oxygen reduction reaction (2e ORR) represents a green alternative to the energy-intensive anthraquinone process. However, the practical application of this method is limited by the lack of cost-effective and high-performance electrocatalysts. Reported here is a hybrid catalyst composed of nickel (Ni) clusters immobilized onto the surface of two-dimensional siloxene nanosheets (Ni/siloxene), which exhibits excellent efficiency and selectivity in electrocatalytic oxygen reduction to H2O2 in an alkaline medium, demonstrating a standard 2e pathway with >95% H2O2 selectivity across a wide potential range. Experimental results disclose that the high performance of Ni/siloxene can be traced to a synergy of the Ni clusters and the oxygen-rich surface of siloxene. Density functional theory (DFT) calculations further reveal a weakened interaction between Ni/siloxene and *OOH and the consequently reduced energy barrier for the *OOH protonation toward H2O2 desorption, thus leading to a high 2e ORR reactivity and selectivity. This work provides a valuable and practical guidance for designing high-performance 2e ORR electrocatalysts based on the rational engineering of the metal–support interaction.

Graphical abstract: Ni clusters immobilized on oxygen-rich siloxene nanosheets for efficient electrocatalytic oxygen reduction toward H2O2 synthesis

Supplementary files

Article information

Article type
Paper
Submitted
31 Dec 2023
Accepted
07 Feb 2024
First published
09 Feb 2024

Dalton Trans., 2024,53, 4823-4832

Ni clusters immobilized on oxygen-rich siloxene nanosheets for efficient electrocatalytic oxygen reduction toward H2O2 synthesis

H. Hu, K. Ma, Y. Yang, N. Jin, L. Zhang, J. Qian and L. Han, Dalton Trans., 2024, 53, 4823 DOI: 10.1039/D3DT04389D

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