Importance of surface carbide formation on the activity and selectivity of Pd surfaces in the selective hydrogenation of acetylene

Yang, Bo; Burch, Robbie; Hardacre, Christopher; Hu, Pei; Hughes, Philip

doi:10.1016/j.susc.2015.07.015

Cited by 45 publications

(37 citation statements)

References 53 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…The first is that the activation energy of ethylene hydrogenation to ethane is larger than that of acetylene hydrogenation to ethylene. Another is the difference between the activation energy of ethylene hydrogenation to ethane (E a ) and the desorption energy of ethylene (|E ad |): ∆E = E a − |E ad |, the larger difference represent the higher the selectivity of ethylene [39][40][41]. The activation energy of ethylene hydrogenation before S doping is 38.88 kcal/mol, which is larger than that of acetylene hydrogenation to ethylene (21.53 kcal/mol), and the selectivity is 15.4 kcal/mol according to the second method.…”

Section: Comparison Of Activity and Selectivity Before And After Dopimentioning

confidence: 99%

A DFT Study of Acetylene Hydrogenation Catalyzed by S-Doped Pd1/g-C3N4

Kang

Zhao

2019

Catalysts

View full text Add to dashboard Cite

To exploit the excellent properties of g-C 3 N 4 , more and more studies have been carried out in various fields in recent years to improve the selectivity of catalysts, especially for selective acetylene hydrogenation. To our best knowledge, Pd catalyst is of great importance to hydrogenate acetylene in ethylene feed. Though we have explored the hydrogenation of acetylene catalyzed by Pd 1 /g-C 3 N 4 before, doping with non-metals has never been studied. In this work, the mechanisms of selective hydrogenation of acetylene to ethylene on S-doped Pd 1 /g-C 3 N 4 were investigated and we also compared this result with undoped Pd 1 /g-C 3 N 4 . By comparing the activation energy and selectivity of undoped Pd 1 /g-C 3 N 4 with those of S-doped C and N sites of Pd 1 /g-C 3 N 4 , we found that S-doped C sites can improve the reactivity, but with a poor selectivity, while the activity of S atom doped N sites was not improved, but the selectivity has improved. Our work provides significant insights to explore the development of high efficiency non-metallic doping single metal atoms supported on 2D layered materials.

show abstract

Section: Comparison Of Activity and Selectivity Before And After Dopimentioning

confidence: 99%

A DFT Study of Acetylene Hydrogenation Catalyzed by S-Doped Pd1/g-C3N4

Kang

Zhao

2019

Catalysts

View full text Add to dashboard Cite

show abstract

“…Plenty of investigations have demonstrated that the partial hydrogenation of acetylene is a structure‐sensitive reaction for Pd, during which the different exposed facets result in the generation of various types of C 2 intermediates that then lead to hydrogenation products such as ethylene, ethane, butylene, and other byproducts. Experimental and theoretical results have revealed that the Pd (1 0 0) facets exhibit better ethylene selectivity than the Pd (1 1 1) facets in acetylene hydrogenation . Kim and co‐workers reported that a cubic Pd catalyst with exposed (1 0 0) facets exhibited a higher acetylene conversion and higher selectivity towards ethylene than a spherical Pd catalyst .…”

Section: Figurementioning

confidence: 99%

“…They ascribed the enhanced selectivity to weak adsorption of multiply bound C 2 species on the (1 0 0) surface. Yang and co‐workers found that Pd (1 0 0) facets in the carbide form generated higher activity and selectivity than the Pd (1 1 1) facets on the basis of density functional theory calculations …”

Section: Figurementioning

confidence: 99%

“…So, in the partial hydrogenation of acetylene the flat Pd (1 0 0) surface can turn into a stepped surface after a long reaction time. The selectivity toward ethylene also decreases with changes in the surface, and this is consistent with previous theoretical and experimental results indicating that the Pd (1 0 0) facet has better selectivity than the (1 1 1) and (211) facets …”

Section: Figurementioning

confidence: 99%

See 1 more Smart Citation

Correlation between Microstructure Evolution of a Well‐Defined Cubic Palladium Catalyst and Selectivity during Acetylene Hydrogenation

et al. 2017

View full text Add to dashboard Cite

The varied surface structures of a Pd catalyst showed different catalytic performances in the partial hydrogenation of acetylene. The exposed Pd (1 0 0) facet is considered to be the most selective of all other facets for the formation of ethylene, but it is unstable and the fine structure needs to be revealed during the reaction. Herein, the evolution of the surface structure of cubic Pd nanoparticles, which are all bound with (1 0 0) facets, was studied by transmission electron microscopy in the partial hydrogenation of acetylene. Furthermore, the relation between the varying surface structure and the activity/selectivity was correlated. The (1 0 0) facets of Pd were transformed into stepped facets during the reaction, derived by adsorption/desorption of the reactants and energy compensation, which was the main reason for the decrease in the selectivity towards ethylene.

show abstract

“…[6] As a catalyst for acetylene hydrogenation, experimental and theoretical results revealed that Pd (100) facets do exhibit higher conversion and better ethylene selectivity than Pd (111) facets. [7,8,9,10] Also, recent papers reported such a faceting-dependent effect namely higher catalytic performances of Pd nanocrystals enclosed by (100) facets compared to those enclosed by (111) facets for formic acid oxidation and furan hydrogenation reactions. [11,12] Otherwise, (111) faceted palladium was found to display a higher activity than (100) faceted one in selective alkyne hydrogenation.…”

Section: Introductionmentioning

confidence: 99%

A New Methodology for Quantifying the Surface Crystallography of Particles from their Tomographic Reconstruction: Application to Pd Nanoparticles Embedded in a Mesoporous Silica Shell

et al. 2020

View full text Add to dashboard Cite

In this work, we propose an experimental approach allowing for the identification and the subsequent quantification of nanoparticles crystallographic facets, based on 3D data obtained using Transmission Electron Microscopy (TEM). The particle shape and faceting can be determined using Electron Tomography (ET) combined with High‐Resolution TEM (HR‐TEM). The quantitative analysis of faceting is carried out on the particles 3D models using a geometrical approach that automatically detects planar regions on particle boundaries. In order to check the reliability of our approach, we analyzed palladium particles confined inside or located at the outer surface of a mesoporous silica shell (Pd@SiO2) after an annealing treatment at 250 °C under hydrogen for 12 hours. From the materials perspective, the aim of the current work is to investigate the encapsulation effect of silica (SiO2) shells on the change in morphology and faceting of palladium nanoparticles during such annealing treatment.

show abstract

Importance of surface carbide formation on the activity and selectivity of Pd surfaces in the selective hydrogenation of acetylene

Cited by 45 publications

References 53 publications

A DFT Study of Acetylene Hydrogenation Catalyzed by S-Doped Pd1/g-C3N4

A DFT Study of Acetylene Hydrogenation Catalyzed by S-Doped Pd1/g-C3N4

Correlation between Microstructure Evolution of a Well‐Defined Cubic Palladium Catalyst and Selectivity during Acetylene Hydrogenation

A New Methodology for Quantifying the Surface Crystallography of Particles from their Tomographic Reconstruction: Application to Pd Nanoparticles Embedded in a Mesoporous Silica Shell

Contact Info

Product

Resources

About