Phase transition in the adsorption process of N-dansylglycinate anion on mercury

Benedetti, L.; Borsari, Marco; Gavioli, G. Battistuzzi; Fontanesi, Claudio

doi:10.1016/0022-0728(90)85187-a

Journal of Electroanalytical Chemistry and Interfacial Electroc

1990

DOI: 10.1016/0022-0728(90)85187-a

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Phase transition in the adsorption process of N-dansylglycinate anion on mercury

L. Benedetti¹,

Marco Borsari²,

G. Battistuzzi Gavioli³

et al.

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Cited by 7 publications

(1 citation statement)

References 12 publications

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“…Often, the mercury-ion-containing salts adhere firmly to the mercury surface in the form of highly insoluble compact monolayers or multilayers. Although the mechanism of their formation has been much investigated (4,5,10,11,13,(17)(18)(19)(20)(21)(22)(23)(24), structural information for these layers on mercury is limited except for the simplest cases, such as Hg 2 Cl 2 (25, 26). The growth of two-dimensional crystals of salts of other metals on mercury surface is known (27, 28), and nucleation and growth phenomena in electrocrystallization have been reviewed recently (29).…”

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confidence: 99%

Self-assembly of a metal-ion-bound monolayer of trigonal connectors on mercury: An electrochemical Langmuir trough

Varaksa

Pospı́šil

Magnera

et al. 2002

Proc. Natl. Acad. Sci. U.S.A.

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The adsorption of the trigonal connector, 1,3,5-tris[10-(3-ethylthiopropyl)dimethylsilyl-1,10-dicarba-closo-decaboran-1-yl]benzene (1), from acetonitrile͞0.1 M LiClO 4 on the surface of mercury at potentials ranging from ؉0.3 to ؊1.4 V (vs. aqueous AgͦAgClͦ1 M LiCl) was examined by voltammetry, Langmuir isotherms at controlled potentials, and impedance measurements. No adsorption is observed at potentials more negative than ϳ ؊0.85 V. Physisorption is seen between ϳ ؊0.85 and 0 V. At positive potentials, adsorbate-assisted anodic dissolution of mercury occurs and an organized surface layer is formed. Although the mercury cations are reduced at ؊0.10 V, the surface layer remains metastable to potentials as negative as ؊0.85 V. Its surface areas per molecule and per redox center are compatible with a regular structure with the connectors 1 woven into a hexagonal network by RRS3 Hg 2 2؉ 4SRR or RRS3 Hg 2؉ 4SRR bridges. The structure is simulated closely by geometry optimization in the semiempirical AM1 approximation. E lsewhere in this issue (1) we outline the motivation for our efforts to prepare extended regular grids on the surface of mercury by reversible self-assembly. Here, we describe an electrochemical Langmuir trough for the determination of a surface molecular area at the interface of mercury and an electrolyte solution at a controlled potential. We use it to shed light on the possible formation of a two-dimensional hexagonal grid by the binding of trigonal connectors to each other through a mutual coupling of their thioether-containing arm terminals by means of ligation to mercury cations.It has been long known (2) that anodic dissolution of mercury is facilitated by the presence of species with a large affinity for mercury ions. These can be anions, such as oxalate (3, 4), or neutral ligands, such as azaaromatics (5). Sulfur compounds, especially sulfide and thiols, have attracted particular attention (6-16). Often, the mercury-ion-containing salts adhere firmly to the mercury surface in the form of highly insoluble compact monolayers or multilayers. Although the mechanism of their formation has been much investigated (4,5,10,11,13,(17)(18)(19)(20)(21)(22)(23)(24), structural information for these layers on mercury is limited except for the simplest cases, such as Hg 2 Cl 2 (25, 26). The growth of two-dimensional crystals of salts of other metals on mercury surface is known (27, 28), and nucleation and growth phenomena in electrocrystallization have been reviewed recently (29). The mercury-adsorbed layers are compact, with lateral interactions among the adsorbed species essential for stability.We have reported (30) the formation of such an adsorbed layer on a dropping mercury electrode from acetonitrile and dichloromethane solutions of a trigonal connector with a thioether link in each of its three arms, and suggested an open hexagonal grid structure for it. We now examine in more detail the properties of a monolayer formed from a similar connector that differs only by substitution of 10-vertex for 12-v...

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mentioning

confidence: 99%

Self-assembly of a metal-ion-bound monolayer of trigonal connectors on mercury: An electrochemical Langmuir trough

Varaksa

Pospı́šil

Magnera

et al. 2002

Proc. Natl. Acad. Sci. U.S.A.

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On the Nature of the Nonanoic Acid Monolayer Adsorbed at the Hg/Aqueous Solution Interface: Influence of Conformational Freedom in Bulk Aqueous Solution

Bordi

Carlà

Passamonti

et al. 1995

Ber Bunsenges Phys Chem

Self Cite

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The adsorption of the nonanoic acid at the electrified Hghqueous solution interface is studied by means of capacity and surface tension measurements. Comparison of the experimental r,,, value with the calculated more favoured solvated conformation suggests that the acid is adsorbed in a partially coiled conformation. The adsorption free energy here determined, together with previously reported values found in the literature concerning other saturated acids and alcohols, is compared with reactivity and calculated molecular descriptors. The collected evidence suggests that the hydrophobic nature of the acid is responsible for the adsorption, while the electric field/molecule interaction, occurring at the electrified interface, governs the desorption. Lastly, some experimental (capacitive transients, effect of the temperature on the tensammetric curves) and theoretical findings are discussed which indicate that the adsorbed acid monolayer should be regarded as a usual, in the field of adsorption at electrodes, disordered network. Thus excluding the occurrence of a two-dimensional phase transition involving the formation of a 2 D solid-like film.

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On the 2D phase transition of adenine adsorbed at the mercury/ethylene glycol solution interface

Benedetti

Camurri

Fontanesi

et al. 2004

Electrochimica Acta

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Phase transition in the adsorption process of N-dansylglycinate anion on mercury

Cited by 7 publications

References 12 publications

Self-assembly of a metal-ion-bound monolayer of trigonal connectors on mercury: An electrochemical Langmuir trough

Self-assembly of a metal-ion-bound monolayer of trigonal connectors on mercury: An electrochemical Langmuir trough

On the Nature of the Nonanoic Acid Monolayer Adsorbed at the Hg/Aqueous Solution Interface: Influence of Conformational Freedom in Bulk Aqueous Solution

On the 2D phase transition of adenine adsorbed at the mercury/ethylene glycol solution interface

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