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Mono and dual hetero-structured M@poly-1,2 diaminoanthraquinone (M = Pt, Pd and Pt-Pd) catalysts for the electrooxidation of small organic fuels in alkaline medium.

ABSTRACT: Oxidation of some small organic fuels such as methanol (MeOH), ethanol (EtOH) and ethylene glycol (EG) was carried out in an alkaline medium using palladium (Pd)-platinum (Pt) nanoparticles/poly1,2-diaminoanthraquinone/glassy carbon (p1,2-DAAQ/GC) catalyst electrodes. Pd and Pt were incorporated into the p1,2-DAAQ/GC electrode using the cyclic voltammetry (CV) technique. The obtained Pd/p1,2-DAAQ/GC, Pt/p1,2-DAAQ/GC, Pt/Pd/p1,2-DAAQ/GC and Pd/Pt/p1,2-DAAQ/GC nanocatalyst electrodes were characterized by scanning electron microscopy (SEM), energy dispersive X-ray spectroscopy (EDX) and CV methods. Real active surface area (A _real) achieved by carbon monoxide (CO) adsorption using differential electrochemical mass spectroscopy (DEMS) technique. The electrochemical activity was evaluated and normalized to A _real per metal loading mass. The electrocatalytic oxidation of the small organic fuels at the prepared nanocatalyst electrodes was studied in 1.0 M NaOH solutions by CV and chronoamperometric (CA) techniques. Pt/Pd/p1,2-DAAQ/GC nanocatalyst electrode exhibited enhanced catalytic activity, better durability and higher tolerance to carbon monoxide generated in the oxidation reaction when compared with the other three studied nanocatalysts. The present investigation suggests that the studied nanocatalysts can be successfully applied in direct oxidation of small organic fuels, especially MeOH.

SUBMITTER: Hathoot AA

PROVIDER: S-EPMC9059733 | biostudies-literature | 2019 Jan

REPOSITORIES: biostudies-literature

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Mono and dual hetero-structured M@poly-1,2 diaminoanthraquinone (M = Pt, Pd and Pt-Pd) catalysts for the electrooxidation of small organic fuels in alkaline medium.

Hathoot Abla Ahmed AA Hassan Khalid Mahmoud KM Ali Asmaa Galal AG Shatla Ahmed Said AS Baltruschat Helmut H Abdel-Azzem Magdi M

RSC advances 20190115 4

Oxidation of some small organic fuels such as methanol (MeOH), ethanol (EtOH) and ethylene glycol (EG) was carried out in an alkaline medium using palladium (Pd)-platinum (Pt) nanoparticles/poly1,2-diaminoanthraquinone/glassy carbon (p1,2-DAAQ/GC) catalyst electrodes. Pd and Pt were incorporated into the p1,2-DAAQ/GC electrode using the cyclic voltammetry (CV) technique. The obtained Pd/p1,2-DAAQ/GC, Pt/p1,2-DAAQ/GC, Pt/Pd/p1,2-DAAQ/GC and Pd/Pt/p1,2-DAAQ/GC nanocatalyst electrodes were characte ...[more]

PMID: 35516099

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Project description:Density functional theory (DFT) and measurements of rate are used to provide evidence for the rate determining step (RDS) and requirements of the active site for CH4 combustion on Pd-Pt bimetallic catalysts in five different distinct kinetic regimes. These five regimes exhibit different rate equations for methane combustion due to the reaction rate constants and diverse dominant adsorbed species for these different kinetically relevant steps. Oxygen chemical potential at the Pd-Pt surface was replaced by oxygen pressure, reflecting the kinetic coupling between C-H and O[double bond, length as m-dash]O bond cleavage steps. C-H bond cleavage occurs on different active sites in five of these kinetic regimes, evolving from vacancy-vacancy (*-*) to oxygen-vacancy (O*-*), oxygen-oxygen (O*-O*) site pairs, monolayer Pd-O, and ultimately to oxide bulk with Pd-O site pairs as the oxygen chemical potential increases. It is easier to form a metallic surface at low oxygen pressure, implying minimal O* coverage. The sole kinetically relevant step on uncovered Pd-Pt surfaces for methane combustion is O[double bond, length as m-dash]O bond cleavage. The supply of oxygen is obviously more important than the supply of methane in regime (I). As vacancies become less available on metallic surfaces, C-H bond cleavage occurs via O*-* paired sites, the energy barrier of which is much higher than that on uncovered Pd-Pt surfaces. In this regime (II), O[double bond, length as m-dash]O bond cleavage is still an irreversible process because O* will be consumed by the rapidly formed products of methane dissociation. For the oxygen saturated surfaces in regime (III), C-H bond cleavage occurs on two adjacent adsorbed oxygens that form OH and weak CH3-O bond interactions, resulting in a low activity for methane combustion. On the oxidation surfaces (IV and V), exposed metal atoms and their adjacent exposed lattice oxygen were the active sites, leading to a large decrease in C-H bond cleavage energy barrier, deduced from both experiment and theory. The increase of the metallic oxide thickness (increase of oxygen potential) increases the methane combustion turnover rates on Pd-Pt catalysts.

Dataset Information

Mono and dual hetero-structured M@poly-1,2 diaminoanthraquinone (M = Pt, Pd and Pt-Pd) catalysts for the electrooxidation of small organic fuels in alkaline medium.

Publications

Mono and dual hetero-structured M@poly-1,2 diaminoanthraquinone (M = Pt, Pd and Pt-Pd) catalysts for the electrooxidation of small organic fuels in alkaline medium.

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