Issue 1, 2024

Regulation of heterogeneous electron transfer reactivity by defect engineering through electrochemically induced brominating addition

Abstract

Enhancing the electrochemical activity of graphene holds great significance for expanding its applications in various electrochemistry fields. In this study, we have demonstrated a facile and quantitative approach for modulating the defect density of single-layer graphene (SLG) via an electrochemically induced bromination process facilitated by cyclic voltammetry. This controlled defect engineering directly impacts the heterogeneous electron transfer (HET) rate of SLG. By utilizing Raman spectroscopy and scanning electrochemical microscopy (SECM), we have established a correlation between the HET kinetics and both the defect density (nD) and mean distance between defects (LD) of SLG. The variation of the HET rate (k0) with the defect density manifested a distinctive three-stage behavior. Initially, k0 increased slightly with the increasing nD, and then it experienced a rapid increase as nD further increased. However, once the defect density surpassed a critical value of about 1.8 × 1012 cm−2 (LD < 4.2 nm), k0 decreased rapidly. Notably, the results revealed a remarkable 35-fold enhancement of k0 under the optimal defect density conditions compared to pristine SLG. This research paves the way for controllable defect engineering as a powerful strategy to enhance the electrochemical activity of graphene, opening up new possibilities for its utilization in a wide range of electrochemical applications.

Graphical abstract: Regulation of heterogeneous electron transfer reactivity by defect engineering through electrochemically induced brominating addition

Supplementary files

Article information

Article type
Edge Article
Submitted
28 iyl 2023
Accepted
08 noy 2023
First published
09 noy 2023
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY-NC license

Chem. Sci., 2024,15, 95-101

Regulation of heterogeneous electron transfer reactivity by defect engineering through electrochemically induced brominating addition

L. Zeng, L. Han, W. Nan, W. Song, S. Luo, Y. Wu, J. Su and D. Zhan, Chem. Sci., 2024, 15, 95 DOI: 10.1039/D3SC03920J

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