Inexpensive activated coke electrocatalyst for high-efficiency hydrogen peroxide production: Coupling effects of amorphous carbon cluster and oxygen dopant

[Display omitted] •Cost-effective activated coke catalyst is prepared towards H2O2 production.•High activity, selectivity and stability are achieved in the typical alkaline system.•The coupling effects of carbon plane size and oxygen doping are evidenced.•A new activity descriptor of Fukui function...

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Bibliographic Details
Published in:Applied catalysis. B, Environmental Environmental, 2021-06, Vol.286, p.119860, Article 119860
Main Authors: Sun, Fei, Yang, Chaowei, Qu, Zhibin, Zhou, Wei, Ding, Yani, Gao, Jihui, Zhao, Guangbo, Xing, Defeng, Lu, Yunfeng
Format: Article
Language:English
Subjects:
Activated carbon
Activated coke
Activity descriptor
Amorphous carbon
Carbon
Carbon dioxide
Catalysts
Clusters
Coke
Control stability
Coupling
Density functional theory
Electrocatalyst
Electrocatalysts
Electrochemistry
Hydrogen peroxide
Lattices
Oxygen
Oxygen functional group
Selectivity
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Summary:[Display omitted] •Cost-effective activated coke catalyst is prepared towards H2O2 production.•High activity, selectivity and stability are achieved in the typical alkaline system.•The coupling effects of carbon plane size and oxygen doping are evidenced.•A new activity descriptor of Fukui function is proposed to reveal active sites. Electrochemical oxygen reduction has been regarded as a promising choice to enable H2O2 on-site production and utilization wherein the exploration of high-efficiency yet cost-effective catalysts is the key. Here, we demonstrate a low-cost activated coke (AC) electrocatalyst with size-tailored amorphous carbon clusters doped by oxygen groups, prepared through a facile CO2 assisted mechanochemistry approach, to deliver among the highest performances reported in a typical alkaline system, including high activity (onset potential of 0.83 V), high H2O2 selectivity (∼90 %) and long-term stability. A series of control experiments, structural characterizations before and after electrochemical tests and density functional theory calculations provide a new insight into the coupling role of carbon cluster size and oxygen doping in H2O2 electrochemical production process, that is, size-reduced amorphous carbon lattices with abundant edges contribute to the high activity, while the basal carbon atoms in ether-doped small-size carbon plane are the most active sites towards H2O2 selectivity.
ISSN:0926-3373
1873-3883
DOI:10.1016/j.apcatb.2020.119860