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- W2074863434 abstract "Interfacial reactions kinetics often differ from kinetics of bulk reactions. Here, we describe how the density change of an immobilized reactant influences the kinetics of interfacial reactions. Self-assembled monolayers (SAMs) of alkanethiolates on gold were used as a model interface and the Diels-Alder reaction between immobilized quinones and soluble cyclopentadiene was used as a model reaction. The kinetic behavior was studied using varying concentrations of quinones. An unusual threshold density of quinones (<TEX>${Gamma}_c$</TEX> = 5.2-7.2%), at which the pseudo-first order rate constant started to vary as the reaction progressed, was observed. This unexpected kinetic behavior was attributed to the phase-separation phenomena of multi-component SAMs. Additional experiments using more phase-separated two-component SAMs supported this explanation by revealing a significant decrease in <TEX>${Gamma}_c$</TEX> values. When the background hydroxyl group was replaced with carboxylic or phosphoric acid groups, <TEX>${Gamma}_c$</TEX> was observed at below 1%. Also, more phase-separated thermodynamically controlled SAMs produced a lower critical density (3% < <TEX>${Gamma}_c$</TEX> < 4.9%) than that of the less phaseseparated kinetically controlled SAMs (6.5% < <TEX>${Gamma}_c$</TEX> < 8.9%)." @default.
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- W2074863434 date "2011-05-20" @default.
- W2074863434 modified "2023-10-02" @default.
- W2074863434 title "Dependence of an Interfacial Diels-Alder Reaction Kinetics on the Density of the Immobilized Dienophile: An Example of Phase-Separation" @default.
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- W2074863434 doi "https://doi.org/10.5012/bkcs.2011.32.5.1679" @default.
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