Insight into the solvent effects on ethanol oxidation on Ir(100)

Wu, Ruitao; Wang, Lichang

doi:10.1039/d2cp04899j

Cited by 11 publications

(7 citation statements)

References 77 publications

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“…52,53 An aspect that deserves an in-depth evaluation in future studies is certainly the role of the solvent in the EOR process. Although the solvent can play a relevant role in the chemical processes occurring in direct EtOH fuel cells, 54 it is often overlooked in quantum mechanical calculations, due to the large computational cost of introducing a significant number of water molecules. Concerning the intermediate reaction 1, we may speculate that the effect of the solvent is to decrease roughly the adsorption energies of the reactants, 28 eventually increasing the average distance between the surface and reactants compared to vacuum.…”

Section: Discussionmentioning

confidence: 99%

Insights into the Rate-Determining Step of the Ethanol Electro-oxidation Reaction on the Pd(111) Surface through Ab Initio Molecular Dynamics Simulations

Campeggio,

Giurlani,

Pagliai

et al. 2023

J. Phys. Chem. C

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The ethanol electro-oxidation mechanism on a Pd(111) surface in alkaline media has been studied through ab initio molecular dynamics simulations. It is known that, under these conditions, ethanol undergoes partial oxidation to acetate and that hydroxylation of the acetyl radical plays a fundamental role in the overall reaction kinetics. Therefore, we focused on this reaction step, specifically addressing the interplay of the acetyl and hydroxyl radicals and especially the effect of their arrangement over the Pd surface on the hydroxylation process. We observed that the strength of the interactions of the reacting species with the Pd surface significantly modulates the propensity of the reaction. In fact, for minimum-energy arrangements of the acetyl-surface and OH-surface systems, hydroxylation appears hindered by the strong interactions between the surface and substrates, while it readily takes place when the substrates are moved away from the surface. These results open to the idea of rational design of cocatalysts based on the tuning of surface chemical properties addressed to weaken the adsorbate/adsorbent interactions, eventually enhancing the exchange current density.

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Section: Discussionmentioning

confidence: 99%

Insights into the Rate-Determining Step of the Ethanol Electro-oxidation Reaction on the Pd(111) Surface through Ab Initio Molecular Dynamics Simulations

Campeggio,

Giurlani,

Pagliai

et al. 2023

J. Phys. Chem. C

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“…Activation of C-H or O-H bond is achieved by photons, which follows different mechanism. 26,27,29,[137][138][139] Co-adsorbate, such as water, 140 or hydrogen bond 141 and solvent effect 142 will be interesting in the future studies to consider. Other areas of interest are to understand the effect of alloy on the adsorption of glycerol as previous studies showing promises of alloying effect, 104,107,108,[143][144][145][146][147] to modulate the oxidative state of the catalysts, 119,148 or to explore the size of nanocatalysts.…”

Section: Discussionmentioning

confidence: 99%

DFT and DFT-D3 Studies of Glycerol Adsorption on the Cu(111), Cu(100), and Cu(110) Surfaces

Drake,

Jayamaha,

Wang

2023

Preprint

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Adsorption of glycerol is the first step in many catalytic reactions to transform glycerol that was formed as biodiesel byproduct into valuable products. Among many feasible catalysts, Cu seems to be a good choice due to its abundance and cost consideration, though extensive studies are needed to evaluate the performance of Cu catalysts on glycerol transformation. Density functional theory (DFT) calculations and van der Waals corrected calculations (DFT-D3) were therefore performed in this work to study the adsorption of glycerol on the three most abundant copper surfaces: Cu(111), Cu(100), and Cu(110). Inclusion of the van der Waals interactions resulted in higher adsorption energies and shorter Cu-O bond distances. The most favorable adsorption location was determined to be the Cu(110) long bridge site. The strongest adsorption is the atop site on the Cu(111) and the hollow site on the Cu(100), though the other adsorption sites are also very favorable.

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“…Many catalytic active nanoparticles of transition metals, such as Pt, 1,2 Pd, [3][4][5] Rh, 6,7 Au, [8][9][10][11] Ir, [12][13][14] and Cun [15][16][17][18][19][20][21][22] have been studied extensively for catalysis as well as other applications. For instance, Ir was studied due to their high activities in ethanol oxidation reaction [23][24][25][26][27][28][29][30][31][32] and Ni for steam reforming of alkanes, [33][34][35][36] Compared to other transition metals, the abundant and cheap Cu has been used as catalysts for ethanol conversation [37][38][39][40][41][42][43][44][45][46][47] and other applications, [48]…”

Section: Introductionmentioning

confidence: 99%

Substrate effect on the structure and properties of Cu clusters supported on ZnO

Love-Nkansah

Jayamaha

Wang

2023

Preprint

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To understand the interaction between the Cu clusters and the ZnO substrate, we performed density functional theory (DFT) calculations on the adsorptions of small copper clusters on the ZnO(100) surface. The PBE functional was used in the DFT calculations with a plane wave basis set. The structural changes of the Cu clusters upon adsorption on the ZnO surface were provided. Although a few different adsorption sites are available, a single Cu atom was found to be adsorbed on three positions on a ZnO(100) surface. The adsorption strength of a Cu dimer is increased with respect to the adsorption of a single Cu atom. In the adsorptions of tetramers, and pentamers, three-dimensional configurations of Cu clusters are more favorable than the planer.

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Insight into the solvent effects on ethanol oxidation on Ir(100)

Abstract: Solvent effect has always been a non-negligible factor for aqueous catalytic reactions, though few studies were devoted towards the molecular understanding and impact of the solvent effects on the catalysis....

Cited by 11 publications

References 77 publications

Insights into the Rate-Determining Step of the Ethanol Electro-oxidation Reaction on the Pd(111) Surface through Ab Initio Molecular Dynamics Simulations

Insights into the Rate-Determining Step of the Ethanol Electro-oxidation Reaction on the Pd(111) Surface through Ab Initio Molecular Dynamics Simulations

DFT and DFT-D3 Studies of Glycerol Adsorption on the Cu(111), Cu(100), and Cu(110) Surfaces

Substrate effect on the structure and properties of Cu clusters supported on ZnO

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