Graph-Based Analysis of Ethylene Glycol Decomposition on a Palladium Cluster

Cortese, Remedios; Schimmenti, Roberto; Ferrante, Francesco; Prestianni, Antonio; Decarolis, Donato; Duca, Dario

doi:10.1021/acs.jpcc.7b00850

Cited by 8 publications

(5 citation statements)

References 45 publications

(72 reference statements)

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Because it is well documented that the H 2 fragmentation on both metal-based and metal-free materials might induce changes in the multiplicity of the system, 22,58 the geometries of the different species were optimized in both singlet and triplet states.…”

Section: H 2 Splitting On Bn Fragmentsmentioning

confidence: 99%

Hydrogen Arrangements on Defective Quasi-Molecular BN Fragments

2019

Self Cite

View full text Add to dashboard Cite

Considering the ever-increasing interest in metal-free materials, some potential chemical applications of quasi-molecular boron nitride (BN) derivatives were tested. Specifically, the behavior of BN fragments was analyzed when given defects, producing local electron density changes, were introduced by using topological engineering approaches. The inserted structural faults were Schottky-like divacancy (BN-d) defects, assembled in the fragment frame by the subtraction of one pair of B and N atoms or Stone–Wales (SW) defects. This study is aimed at highlighting the role of these important classes of defects in BN materials hypothesizing their future use in H2-based processes, related to either (i) H2 activation or (ii) H2 production, from preadsorbed hydrogenated molecular species on BN sites. Here, it has been observed that BN species, embodying SW defects, are characterized by endothermic H2 adsorption and fragmentation phenomena in order to guess their potential use in processes based on the transformation or production of hydrogen. On the contrary, in the presence of BN-d defects, and for reasons strictly related to local structural changes occurring along with the hydrogen rearrangements on the defective BN fragments, a possible use can be inferred. Precautions must be however taken to decrease the material rigidity that could actually decrease the ability of the BN fragment to flatten. This conversely seems to be a necessary requirement to have strong exothermic effects, following the rearrangements of the H2 molecules.

show abstract

Section: H 2 Splitting On Bn Fragmentsmentioning

confidence: 99%

Hydrogen Arrangements on Defective Quasi-Molecular BN Fragments

2019

Self Cite

View full text Add to dashboard Cite

show abstract

“…The surface reactivity is also dependent on the activation of C2 reactants and carbonaceous intermediates on different Pd nanofacets. 28 Therefore, the resulting electrocatalytic activity of Pd nanocrystals may vary to some extent case by case for different oxidation reactions.…”

Section: Chemcomm Accepted Manuscriptmentioning

confidence: 99%

Electrocatalytic oxidation of ethanol and ethylene glycol on cubic, octahedral and rhombic dodecahedral palladium nanocrystals

Chen

Wang

et al. 2018

Chem. Commun.

View full text Add to dashboard Cite

Cubic, octahedral and rhombic dodecahedral Pd nanocrystals were synthesized and examined as nanocatalysts for electro-oxidation of ethanol and ethylene glycol. Combined electrochemical measurements and density functional theory calculations reveal that nanofacet-dependent affinity and reactivity of OH and CO are closely linked to the C2 alcohol oxidation activities, with the highest reactivity found on the Pd nanocubes bounded by {100} facets.

show abstract

“…The advantages of an atomistic approach on tuning catalyst properties are well established. − In particular, computational chemistry, mostly based on density functional theory (DFT), had an enormous impact on the development of zeolite catalytic materials and processes. − As a matter of fact, while Hou et al have investigated, by means of periodic DFT calculations, the stabilization of platinum atoms and/or clusters inside the cavities of medium-size high-silica zeolites (i.e., LTA, SOD, CHA, FAU), to the best of our knowledge, a step-by-step computational approach on platinum clustering inside large pores of aluminosilicates is still missing. In fact, commonly either singly supported platinum atoms or Pt nanoparticles are considered, without giving any idea about their formation yet. − In this context, the present work aims at providing atomistic-level insights on (i) the preferential location of a platinum atom embedded in β-zeolite cages, (ii) the energetics related to platinum atoms’ migration, and (iii) the cluster growth process up to a Pt 3 seed.…”

Section: Introductionmentioning

confidence: 99%

DFT Study of Pt Particle Growth inside β-Zeolite Cages

et al. 2023

Self Cite

View full text Add to dashboard Cite

The preferred location and the corresponding energetics of zeolite-embedded single metal atoms and small metal particles are hot topics within active site optimization and catalyst tuning, even as part of bifunctional materials design. In this context, periodic density functional theory was used to provide insights on the interactions of a platinum atom with the microporous cages of a purely silicious β-zeolite (BEA) framework. Cluster growth was subsequently addressed, up to Pt 3 @BEA systems, following a one-by-one platinum atom addition; platinum migration between cages was taken into account as well. An unbiased approach was employed, which allowed a wide panorama of structures being considered in addition to a thorough analysis in terms of energetics, cluster geometries, and cavity distortions. Calculations revealed that the optimal interaction geometry for a single platinum atom is realized where two strong Pt−O bonds in almost linear arrangement can form, regardless of the cavity involved. This can cause distortions or even breaking of the zeolite structure, a factor which however is not decisive in determining the energetics of systems with two and three platinum atoms. Platinum migration is associated with energy barriers ranging from 100 to 200 kJ mol −1 , depending on the cages. Up to the dimensions considered here, preference for clustering is observed, being the embedded Pt 3 systems in almost all cases energetically favored with respect to isolated atoms within the BEA framework.

show abstract

Graph-Based Analysis of Ethylene Glycol Decomposition on a Palladium Cluster

Cited by 8 publications

References 45 publications

Hydrogen Arrangements on Defective Quasi-Molecular BN Fragments

Hydrogen Arrangements on Defective Quasi-Molecular BN Fragments

Electrocatalytic oxidation of ethanol and ethylene glycol on cubic, octahedral and rhombic dodecahedral palladium nanocrystals

DFT Study of Pt Particle Growth inside β-Zeolite Cages

Contact Info

Product

Resources

About