Issue 4, 2023

Ether-based electrolytes enable the application of nitrogen and sulfur co-doped 3D graphene frameworks as anodes in high-performance sodium-ion batteries

Abstract

The development of graphitic carbon materials as anodes of sodium-ion batteries (SIBs) is greatly restricted by their inherent low specific capacity. Herein, nitrogen and sulfur co-doped 3D graphene frameworks (NSGFs) were successfully synthesized via a simple and facile one-step hydrothermal method and exhibited high Na storage capacity in ether-based electrolytes. A systematic comparison was made between NSGFs, undoped graphene frameworks (GFs) and nitrogen-doped graphene frameworks (NGFs). It is demonstrated that the high specific capacity of NSGFs can be attributed to the free diffusion of Na ions within the graphene layer and reversible reaction between –C–Sx–C– covalent chains and Na ions thanks to the large interplanar distance and the dominant –C–Sx–C– covalent chains in NSGFs. NSGF anodes, therefore, exhibit a high initial coulombic efficiency (ICE) (92.8%) and a remarkable specific capacity of 834.0 mA h g−1 at 0.1 A g−1. Kinetic analysis verified that the synergetic effect of N/S co-doping not only largely enhanced the Na ion diffusion rate but also reduced the electrochemical impedance of NSGFs. Postmortem techniques, such as SEM, ex situ XPS, HTEM and ex situ Raman spectroscopy, all demonstrated the extremely physicochemically stable structure of the 3D graphene matrix and ultrathin inorganic-rich solid electrolyte interphase (SEI) films formed on the surface of NSGFs. Yet it is worth noting that the Na storage performance and mechanism are exclusive to ether-based electrolytes and would be inhibited in their carbonate ester-based counterparts. In addition, the corrosion of copper foils under the synergetic effect of S atoms and ether-based electrolytes was reported for the first time. Interestingly, by-products derived from this corrosion could provide additional Na storage capacity. This work sheds light on the mechanism of improving the electrochemical performance of carbon-based anodes by heteroatom doping in SIBs and provides a new insight for designing high-performance anodes of SIBs.

Graphical abstract: Ether-based electrolytes enable the application of nitrogen and sulfur co-doped 3D graphene frameworks as anodes in high-performance sodium-ion batteries

Supplementary files

Article information

Article type
Paper
Submitted
23 Okt. 2022
Accepted
14 Dec. 2022
First published
15 Dec. 2022

Nanoscale, 2023,15, 1568-1582

Ether-based electrolytes enable the application of nitrogen and sulfur co-doped 3D graphene frameworks as anodes in high-performance sodium-ion batteries

X. Gao, X. Dong, Z. Xing, S. Jamila, H. Hong, H. Jiang, J. Zhang and Z. Ju, Nanoscale, 2023, 15, 1568 DOI: 10.1039/D2NR05885E

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