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Titolo:
Monte Carlo simulation study on the structure and reaction at metal-electrolyte interface. II. Mechanism of nonlinear electrode reactions
Autore:
Goto, N; Kakitani, T; Yamato, T; Hatano, Y;
Indirizzi:
Nagoya Univ, Grad Sch Sci, Dept Phys, Chikusa Ku, Nagoya, Aichi 4648602, Japan Nagoya Univ Nagoya Aichi Japan 4648602 a Ku, Nagoya, Aichi 4648602, Japan Chukyo Univ, Sch Cognit & Comp Sci, Aichi 4700389, Japan Chukyo Univ Aichi Japan 4700389 Cognit & Comp Sci, Aichi 4700389, Japan
Titolo Testata:
JOURNAL OF THE PHYSICAL SOCIETY OF JAPAN
fascicolo: 11, volume: 68, anno: 1999,
pagine: 3729 - 3737
SICI:
0031-9015(199911)68:11<3729:MCSSOT>2.0.ZU;2-J
Fonte:
ISI
Lingua:
ENG
Soggetto:
SCANNING-TUNNELING-MICROSCOPY; MOLECULAR-DYNAMICS SIMULATION; SOLVENT-FREE ENERGIES; COMPUTER-SIMULATION; CHARGED ELECTRODES; AU(111) ELECTRODE; POLAR-SOLVENTS; ADSORPTION; WATER; IONS;
Keywords:
nonlinear electrode reaction; nonlinear fluctuation; metal-electrolyte interface; Helmholtz double layer; electron transfer; energy gap law; electrolyte; central limit theorem; Marcus theory;
Tipo documento:
Article
Natura:
Periodico
Settore Disciplinare:
Physical, Chemical & Earth Sciences
Citazioni:
30
Recensione:
Indirizzi per estratti:
Indirizzo: Kakitani, T Nagoya Univ, Grad Sch Sci, Dept Phys, Chikusa Ku, Furo Cho, Nagoya, Aichi 4648602, Japan Nagoya Univ Furo Cho Nagoya Aichi Japan 4648602 4648602, Japan
Citazione:
N. Goto et al., "Monte Carlo simulation study on the structure and reaction at metal-electrolyte interface. II. Mechanism of nonlinear electrode reactions", J PHYS JPN, 68(11), 1999, pp. 3729-3737

Abstract

Using the two-dimensional free energy surfaces which were obtained previously by the Monte Carlo simulations for metal-electrolyte interfaces by allowing the movement of reactant [N. Goto et al.: J. Phys, Sec. Jpn. 66 (1997)1825], we have analyzed the mechanism of nonlinearity in the electrode reaction in detail. The nonlinearity was defined as a square of ratio between widths of the energy gap laws for the neutralization and ionization reactions. We developed a method to derive the nonlinearity due to only fluctuations of motion of solvent molecules and electrolyte ions for each distance ofthe reactant from the metal surface. We found that the nonlinearity was the largest (4.8) at the distance 6 Angstrom of the reactant from the metal surface, and was the smallest (2.2) at the distance 2 Angstrom where the reactant is in contact with the metal surface and at the distance larger than 9 Angstrom where Gouy-Chapman diffuse layer ends. We also found that the movement of the ions and solvents directly adsorbed to the metal-surface is strongly restricted, showing a feature of dielectric saturation. Combining these facts, we conclude that the strongly adsorbed layer of ions and solvent molecules (Helmholtz double layer) causes a large nonlinear phenomenon ofthe electrode reaction due to breakdown of the central limit theorem especially for the reactant contacting the adsorbed layer.

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Documento generato il 04/04/20 alle ore 11:54:44