Magnesiothermic synthesis of sulfur-doped graphene as an efficient metal-free electrocatalyst for oxygen reduction

Scientific Reports
Jiacheng WangQian Liu

Abstract

Efficient metal-free electrocatalysts for oxygen reduction reaction (ORR) are highly expected in future low-cost energy systems. We have successfully prepared crumpled, sheet-like, sulfur-doped graphene by magnesiothermic reduction of easily available, low-cost, nontoxic CO2 (in the form of Na2CO3) and Na2SO4 as the carbon and sulfur sources, respectively. At high temperature, Mg can reduce not only carbon in the oxidation state of +4 in CO3(2-) to form graphene, but also sulfur in SO4(2-) from its highest (+6) to lowest valence which was hybridized into the carbon sp(2) framework. Various characterization results show that sulfur-doped graphene with only few layers has an appropriate sulfur content, hierarchically robust porous structure, large surface area/pore volume, and highly graphitized textures. The S-doped graphene samples exhibit not only a high activity for ORR with a four-electron pathway, but also superior durability and tolerance to MeOH crossover to 40% Pt/C. This is mainly ascribed to the combination of sulfur-related active sites and hierarchical porous textures, facilitating fast diffusion of oxygen molecules and electrolyte to catalytic sites and release of products from the sites.

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Citations

Dec 3, 2016·Chemical Society Reviews·Xiao-Yu YangBao-Lian Su
Dec 15, 2015·Physical Chemistry Chemical Physics : PCCP·Zhengshan TianChunxiang Xu
Apr 8, 2016·Chemical Society Reviews·Adriano AmbrosiMartin Pumera
Sep 25, 2018·Chemical Society Reviews·Xuecheng YanXiangdong Yao
Mar 17, 2020·Advanced Materials·Wei LiShuangyin Wang
Jul 15, 2016·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Jan LuxaMartin Pumera
Jan 8, 2021·Journal of Biomolecular Structure & Dynamics·Jamelah S Al-OtaibiY Shyma Mary
Mar 9, 2021·ACS Omega·Adyasa Priyadarsini, Bhabani S Mallik
Aug 28, 2020·Chemical Reviews·Zhuxing SunYun Hang Hu

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Methods Mentioned

BETA
scanning electron microscopy
transmission electron microscopy
X-ray

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