Issue 27, 2025

Multilayer graphene crystals with enhanced performances in oxygen reduction and zinc–air batteries via interlayer carbon promoted O[double bond, length as m-dash]O bond dissociation

Abstract

O[double bond, length as m-dash]O bond activation determines activities of oxygen reduction reaction (ORR) catalysts, and developing metal-free catalysts that outperform precious metals remains challenging. Herein, we demonstrate the mechanochemical polymerization of pyrrole tandem carbonization for designing nitrogen-containing, micropore-penetrated multilayer graphene crystals (NM-MGCs) with abundant barrier-free nanochannels for O2, leading to high exposure of carbon atoms adjacent to graphitic nitrogen. Due to the ordered multilayer structure with steady layer-by-layer van der Waals interaction, the resultant exposed interlayer carbon atoms exhibit much improved ability to activate O2 through adsorption-configuration-induced O[double bond, length as m-dash]O bond dissociation in the ORR with approximately zero energy barrier. Thus, the NM-MGCs show record-breaking ORR performance among metal-free catalysts, which can be fabricated as air cathodes for both flow and flexible Zn–air batteries, exhibiting high maximum power density, high specific capacity (815.30 mA h gZn−1 at 5 mA cm−2), and extraordinary long-term cycling durability (>800 h) and round-trip energy efficiency (63.7%). The overall performance of Zn–air batteries assembled using the NM-MGCs surpass those of commercial Pt/C (20 wt%) and many literature-reported metal and/or metal-free electrocatalysts.

Graphical abstract: Multilayer graphene crystals with enhanced performances in oxygen reduction and zinc–air batteries via interlayer carbon promoted O [[double bond, length as m-dash]] O bond dissociation

Supplementary files

Article information

Article type
Edge Article
Submitted
07 Apr 2025
Accepted
05 Jun 2025
First published
11 Jun 2025
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., 2025,16, 12603-12612

Multilayer graphene crystals with enhanced performances in oxygen reduction and zinc–air batteries via interlayer carbon promoted O[double bond, length as m-dash]O bond dissociation

Y. Qu, Q. Tang, D. Wang, B. He, Y. Liu, W. Chen, G. Yu, B. Tang, F. Liu and L. Qu, Chem. Sci., 2025, 16, 12603 DOI: 10.1039/D5SC02570B

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