Cross-Sphere Electrode Reaction: The Case of Hydroxyl Desorption during the Oxygen Reduction Reaction on Pt(111) in Alkaline Media

Author(s):  
Yuke Li ◽  
Zhi-Feng Liu
2021 ◽  
Author(s):  
Yuke Li ◽  
Zhi-Feng Liu

Hydroxide ion is a common electrolyte when electrode reactions take place in alkaline media. In the case of oxygen reduction reaction on Pt(111), we demonstrate by ab initio molecular dynamics calculations, that the desorption of hydroxyl (OH*) from the electrode surface to form a solvated OH<sup>−</sup> is a cross sphere process, with the reactant OH* in the inner sphere and the product OH<sup>−</sup> directly generated in the aqueous outer sphere. Such a mechanism is distinct from the typical inner sphere and outer sphere reactions. It is dictated by the strong hydrogen bonding interactions between a hydroxide ion and water molecules and facilitated by proton transfer through solvation layers. It should play a significant role whenever OH* desorption, or its reverse, OH<sup>−</sup> adsorption, is involved in an electrochemical reaction


2021 ◽  
Author(s):  
Yuke Li ◽  
Zhi-Feng Liu

Hydroxide ion is a common electrolyte when electrode reactions take place in alkaline media. In the case of oxygen reduction reaction on Pt(111), we demonstrate by ab initio molecular dynamics calculations, that the desorption of hydroxyl (OH*) from the electrode surface to form a solvated OH<sup>−</sup> is a cross sphere process, with the reactant OH* in the inner sphere and the product OH<sup>−</sup> directly generated in the aqueous outer sphere. Such a mechanism is distinct from the typical inner sphere and outer sphere reactions. It is dictated by the strong hydrogen bonding interactions between a hydroxide ion and water molecules and facilitated by proton transfer through solvation layers. It should play a significant role whenever OH* desorption, or its reverse, OH<sup>−</sup> adsorption, is involved in an electrochemical reaction


2020 ◽  
Vol 9 (1) ◽  
pp. 843-852
Author(s):  
Hunan Jiang ◽  
Jinyang Li ◽  
Mengni Liang ◽  
Hanpeng Deng ◽  
Zuowan Zhou

AbstractAlthough Fe–N/C catalysts have received increasing attention in recent years for oxygen reduction reaction (ORR), it is still challenging to precisely control the active sites during the preparation. Herein, we report FexN@RGO catalysts with the size of 2–6 nm derived from the pyrolysis of graphene oxide and 1,1′-diacetylferrocene as C and Fe precursors under the NH3/Ar atmosphere as N source. The 1,1′-diacetylferrocene transforms to Fe3O4 at 600°C and transforms to Fe3N and Fe2N at 700°C and 800°C, respectively. The as-prepared FexN@RGO catalysts exhibited superior electrocatalytic activities in acidic and alkaline media compared with the commercial 10% Pt/C, in terms of electrochemical surface area, onset potential, half-wave potential, number of electrons transferred, kinetic current density, and exchange current density. In addition, the stability of FGN-8 also outperformed commercial 10% Pt/C after 10000 cycles, which demonstrates the as-prepared FexN@RGO as durable and active ORR catalysts in acidic media.


ChemSusChem ◽  
2014 ◽  
Vol 7 (12) ◽  
pp. 3356-3361 ◽  
Author(s):  
Zhiming Cui ◽  
Minghui Yang ◽  
Hao Chen ◽  
Mengtian Zhao ◽  
Francis J. DiSalvo

2019 ◽  
Vol 71 ◽  
pp. 234-241 ◽  
Author(s):  
Yun Sik Kang ◽  
Yoonhye Heo ◽  
Jae Young Jung ◽  
Yeonsun Sohn ◽  
Soo-Hyoung Lee ◽  
...  

RSC Advances ◽  
2015 ◽  
Vol 5 (2) ◽  
pp. 1571-1580 ◽  
Author(s):  
Dongyoon Shin ◽  
Beomgyun Jeong ◽  
Myounghoon Choun ◽  
Joey D. Ocon ◽  
Jaeyoung Lee

An optimal catalyst testing methodology that could allow precise benchmarking to obtain standardized ORR activity is put forward.


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