A density functional theory study of partial oxidation of propylene on Cu 2 O(0  0  1) and CuO(0  0  1) surfaces

Düzenli, Derya; Atmaca, Deniz Onay; Gezer, Miray Gülbiter; Önal, Işık

doi:10.1016/j.apsusc.2015.07.155

Cited by 41 publications

(17 citation statements)

References 59 publications

(88 reference statements)

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Other interesting catalytic systems that have attained the attention of some theoretical studies include the catalytic behavior of immobilized NiO nanoparticles [124]; the epoxidation of propylene on the surface of CuO, which has been studied by Düzenli et al [125] using plane-wave DFT; the use of palladium(II) complexes in the epoxidation of olefins [126,127]; and also the epoxidation of ethylene using a bi-metallic palladium-silver catalyst [128].…”

Section: Other Epoxidation Catalysts: a Brief Overviewmentioning

confidence: 99%

Strengths, Weaknesses, Opportunities and Threats: Computational Studies of Mn- and Fe-Catalyzed Epoxidations

Teixeira

Cordeiro

2016

Catalysts

View full text Add to dashboard Cite

Abstract:The importance of epoxides as synthetic intermediates in a number of highly added-value chemicals, as well as the search for novel and more sustainable chemical processes have brought considerable attention to the catalytic activity of manganese and iron complexes towards the epoxidation of alkenes using non-toxic terminal oxidants. Particular attention has been given to Mn(salen) and Fe(porphyrin) catalysts. While the former attain remarkable enantioselectivity towards the epoxidation of cis-alkenes, the latter also serve as an important model for the behavior of cytochrome P450, thus allowing the exploration of complex biological processes. In this review, a systematic survey of the bibliographical data for the theoretical studies on Mn-and Fe-catalyzed epoxidations is presented. The most interesting patterns and trends are reported and finally analyzed using an evaluation framework similar to the SWOT (Strengths, Weaknesses, Opportunities and Threats) analysis performed in enterprise media, with the ultimate aim to provide an overview of current trends and areas for future exploration.

show abstract

Section: Other Epoxidation Catalysts: a Brief Overviewmentioning

confidence: 99%

Strengths, Weaknesses, Opportunities and Threats: Computational Studies of Mn- and Fe-Catalyzed Epoxidations

Teixeira

Cordeiro

2016

Catalysts

View full text Add to dashboard Cite

show abstract

“…According to He et al., Cu + centers act as active species by providing electrophilic oxygen for propene epoxidation . DFT studies confirmed these assumptions by calculating an easier formation of PO on Cu 2 O than on CuO . CuO/SBA‐15 samples may contain minor amounts of Cu + centers at the surface under reaction conditions.…”

Section: Resultsmentioning

confidence: 68%

Correlation between Copper Oxide Particle Size and Selectivity towards Propylene Oxide in Selective Oxidation of Propene

et al. 2018

View full text Add to dashboard Cite

Copper oxide catalysts supported on nanostructured silica SBA‐15 were synthesized with varying copper loadings in a range from 1.1 to 19.4 wt.%. Catalysts were structurally characterized by N2 physisorption, X‐ray diffraction and ex situ as well as in situ diffuse reflectance UV‐Vis spectroscopy. Copper oxide species contained Cu2+ in an octahedral configuration with a tetragonal distortion. Increasing the copper loading resulted in a decreasing optical band gap, which is associated with a growing particle size. Additionally, CuO/SBA‐15 samples were examined by temperature‐programmed reduction confirming a narrow particle size distribution. Structural evolution and catalytic activity were investigated during selective oxidation of propene focusing on product distribution of nucleophilic and electrophilic oxidation. Catalytic testing was carried out using an on‐line GC and MS coupled to a laboratory fixed‐bed reactor. All catalysts selectively oxidized propene to acrolein and propylene oxide (PO). With time on stream activity decreased while selectivity towards acrolein and PO increased. While selectivity towards PO increased with copper loading and, hence, copper oxide particle size, selectivity towards acrolein was largely independent of copper loading.

show abstract

“…Due to the inherently larger number of atoms in solid state structures (and imposed periodic boundary conditions), the calculation times are usually longer compared to molecular systems. If we again take the example of propylene epoxidation, for which Cu 2 O is a potential catalyst [338][339][340], we can estimate the total computing time based on the time required for a single calculation of a (001) slab with an extension of 2 × 2 × 3 , which can be taken as the minimal slab size for the exploration of such a reaction. This then leads to a total computing time of 10 6 − 10 7 years on a single core.…”

Section: Resource Estimates For Automated Exploration Of Heterogeneou...mentioning

confidence: 99%

Autonomous Reaction Network Exploration in Homogeneous and Heterogeneous Catalysis

Steiner

Reiher

2022

Top Catal

View full text Add to dashboard Cite

Autonomous computations that rely on automated reaction network elucidation algorithms may pave the way to make computational catalysis on a par with experimental research in the field. Several advantages of this approach are key to catalysis: (i) automation allows one to consider orders of magnitude more structures in a systematic and open-ended fashion than what would be accessible by manual inspection. Eventually, full resolution in terms of structural varieties and conformations as well as with respect to the type and number of potentially important elementary reaction steps (including decomposition reactions that determine turnover numbers) may be achieved. (ii) Fast electronic structure methods with uncertainty quantification warrant high efficiency and reliability in order to not only deliver results quickly, but also to allow for predictive work. (iii) A high degree of autonomy reduces the amount of manual human work, processing errors, and human bias. Although being inherently unbiased, it is still steerable with respect to specific regions of an emerging network and with respect to the addition of new reactant species. This allows for a high fidelity of the formalization of some catalytic process and for surprising in silico discoveries. In this work, we first review the state of the art in computational catalysis to embed autonomous explorations into the general field from which it draws its ingredients. We then elaborate on the specific conceptual issues that arise in the context of autonomous computational procedures, some of which we discuss at an example catalytic system. Graphical Abstract

show abstract

A density functional theory study of partial oxidation of propylene on Cu 2 O(0 0 1) and CuO(0 0 1) surfaces

Cited by 41 publications

References 59 publications

Strengths, Weaknesses, Opportunities and Threats: Computational Studies of Mn- and Fe-Catalyzed Epoxidations

Strengths, Weaknesses, Opportunities and Threats: Computational Studies of Mn- and Fe-Catalyzed Epoxidations

Correlation between Copper Oxide Particle Size and Selectivity towards Propylene Oxide in Selective Oxidation of Propene

Autonomous Reaction Network Exploration in Homogeneous and Heterogeneous Catalysis

Contact Info

Product

Resources

About