Issue 1, 2021

Nitrogen and oxygen tailoring of a solid carbon active site for two-electron selectivity electrocatalysis

Abstract

The synthesis of hydrogen peroxide (H2O2) via two-electron (2eāˆ’) oxygen reduction reaction (ORR) electrocatalysis has garnered extensive attention as an appealing green and safe production technology. However, the key progress is still strongly dependent on developing highly active, selective and stable electrocatalysts. Here, guided by first-principles calculations, we developed a rational design for nitrogen (N) and oxygen (O) tailoring of carbon materials by precisely controlling the pyridinic N (Pydn-N) structure and the oxygen doping. The second nearest C atoms of Pydn-N were identified to be the active site, and this is suppressed owing to its local chemical environment and increase in the oxygen dopant content. Experimentally, high-temperature hydrogenation (HTH) regulates the Pydn-N content and synchronous oxygen removal for N,O co-doped carbons (CNO-x). The increment of Pydn-N from 37.42% up to 39.73%, along with oxygen removal from 5.24 at% down to 3.80 at% after HTH, promotes the H2O2 selectivity and electron transfer number (n) to 82% and 2.36. The H2O2 production rate is stable at around 200 mmol gcatāˆ’1 hāˆ’1 and a faradaic efficiency (F.E.) of up to 80% was recorded during the initial 4 h. The long-term H2O2 production further highlights the significance of sustaining the Pydn-N structure, modulating the solid carbon active site.

Graphical abstract: Nitrogen and oxygen tailoring of a solid carbon active site for two-electron selectivity electrocatalysis

Supplementary files

Article information

Article type
Research Article
Submitted
10 Sep 2020
Accepted
29 Oct 2020
First published
29 Oct 2020

Inorg. Chem. Front., 2021,8, 173-181

Nitrogen and oxygen tailoring of a solid carbon active site for two-electron selectivity electrocatalysis

H. Shao, Q. Zhuang, H. Gao, Y. Wang, L. Ji, X. Wang, T. Zhang, L. Duan, J. Bai, Z. Niu and J. Liu, Inorg. Chem. Front., 2021, 8, 173 DOI: 10.1039/D0QI01089H

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