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Fe-Treated Heteroatom (S/N/B/P)-Doped Graphene Electrocatalysts for Water Oxidation
- Fe-Treated Heteroatom (S/N/B/P)-Doped Graphene Electrocatalysts for Water Oxidation
- Razmjooei, Fatemeh; Singh, Kiran Pal; Yang, Dae-Soo; Cui, Wei; Jang, Yun Hee; Yu, Jong-Sung
- DGIST Authors
- Jang, Yun Hee; Yu, Jong-Sung
- Issue Date
- ACS Catalysis, 7(4), 2381-2391
- Article Type
- Bi Functional Electrocatalyst; Catalyst; Catalyst Activity; Catalyst Surfaces; Catalysts; Chemical Bonds; Chemical Equations; Density Functional Theory; Desorption; Efficient Electrocatalyst; Electrocatalysis; Electrocatalysis; Electrocatalysts; Electronegativity; Free Energy; Graphene; Heteroatom Doping; Heteroatoms; Iron; Iron; Long Term Stability; Nitrogen; Number of Active Sites; Oxide; Oxygen Evolution Reaction; Oxygen Evolution Reaction; Oxygen Evolution Reaction; Phosphorus; Reduced Graphene Oxide (RGO); Reduced Graphene Oxides (RGO); Reduced Graphene Oxides (RGO); Reduction Reaction; Sulfur Doped Graphene; Walled Carbon Nanotubes
- Anodic water splitting is driven by hydroxide (OH-) adsorption on the catalyst surface and consequent O2 desorption. In this work, various heteroatoms (S/N/B/P) with different electronegativities and oxophilicities are introduced to alter the catalytic activity of reduced graphene oxide (RGO) as a catalyst for the oxygen evolution reaction (OER). It is found that, surprisingly, S-doped RGO outperforms the other RGOs doped with more electropositive or electronegative and more oxophilic heteroatoms, and this effect becomes more prominent after Fe treatment of the respective catalysts. Herein, we evaluate the OER activity of a series of Fe-treated mono-heteroatom (S/N/B/P)-doped RGO (Fe-X-G) catalysts, among which interestingly S-doped RGO catalyst treated with Fe (Fe-S-G) is found to show better OER activity than the well-known active Fe-N-C catalyst, demonstrating the best activity among all of the prepared catalysts, close to that of the state of the art IrO2/C catalyst, along with pronounced long-term stability. Density functional theory (DFT) calculations indicate that the OER activity highly depends on the electroneutrality and oxophilicity of doped heteroatoms and doping-induced charge distribution over RGO, demonstrating that S with mediocre electronegativity and the least oxophilicity exhibits optimal free energy for the adsorption of the OER intermediate and desorption of the final OER product. Furthermore, it is found that Fe treatment greatly helps in enhancing the number of active sites through the regeneration of reduced catalytically active S sites and improving the conductivity and surface area of the S-doped RGO, which are found to be key factors to furnish the Fe-S-G catalyst with the capability to catalyze the OER with high efficiency, even though Fe is found to be absent in the final catalyst. (Chemical Equation Presented). © 2017 American Chemical Society.
- American Chemical Society
- Related Researcher
Light, Salts and Water Research Group
Materials chemistry; nanomaterials; electrochemistry; carbon and porous materials; fuel cell; battery; supercapacitor; sensor and photochemical catalyst
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- Department of Energy Science and EngineeringLight, Salts and Water Research Group1. Journal Articles
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