DFT study of Hg adsorption on M-substituted Pd(1 1 1) and PdM/γ-Al 2 O 3 (1 1 0) (M = Au, Ag, Cu) surfaces

Wang, Jiancheng; Yu, Hao; Geng, Lu Yang; Liu, Jianwen; Han, Lupeng; Chang, Liping; Feng, Gang; Ling, Lixia

doi:10.1016/j.apsusc.2015.07.086

Cited by 13 publications

(4 citation statements)

References 45 publications

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“…The coordination number of each Al atom was expressed by subscript. As has been described in many previous works [33,34], the Al atoms in bulk -alumina are in tetrahedral and octahedron sites. After cleavage, the tetrahedral and octahedron Al atoms expose as the tricoordinated and tetracoordinated Al, respectively, in the (110) surface.…”

Section: Computational Detailsmentioning

confidence: 77%

Density Functional Theory Investigation into the B and Ga Doped Clean and Water Covered γ-Alumina Surfaces

Cheng

et al. 2017

Journal of Chemistry

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The structures and energies of the B and Ga incorporated -alumina surface as well as the adsorption of water are investigated using dispersion corrected density functional theory. The results show that the substitution of surface Al atom by B atom is not so favored as Ga atom. The substitution reaction prefers to occur at the tricoordinated A(4) sites. However, the substitution reaction becomes less thermodynamically favored when more Al atoms are substituted by B and Ga atoms on the surface. Moreover, the substitution of bulk Al atoms is not so favored as the Al atoms by B and Ga on the surface. The -alumina surface is found to have stronger adsorption ability for water than the B and Ga incorporated surface. The total adsorption energy increases as water coverage increases, while the stepwise adsorption energy decreases. The studies show the coverage of water at 7.5 H 2 O/nm 2 (five H 2 O molecules per unit cell) can fully cover the active sites and the further water molecule could only be physically adsorbed on the surface.

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Section: Computational Detailsmentioning

confidence: 77%

Density Functional Theory Investigation into the B and Ga Doped Clean and Water Covered γ-Alumina Surfaces

Cheng

et al. 2017

Journal of Chemistry

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“…The adsorption of Hg 0 was calculated to be stronger on the step and vacancy-defective Pd(1 1 1) surface as compared to the perfect Pd(1 1 1) surface . Also, the binding of Hg 0 on Pd/γ-Al 2 O 3 was calculated to be stronger than its binding on the pure γ-Al 2 O 3 surface. , …”

Section: Introductionmentioning

confidence: 94%

“…DFT calculations were performed to evaluate the adsorption of Hg 0 on the surfaces of Pd/γ-Al 2 O 3 , bimetallic PdM/γ-Al 2 O 3 (M = Au, Ag, Cu), and homogeneous Pd-based alloys, viz., Ag 3 Pd , AgPd 3 , Au 3 Pd, AuPd 3 , Cu 3 Pd, and CuPd 3. ,, It was shown that the bimetallic compositions could result in a stronger Hg 0 adsorption as compared to the individual component metals, and was attributed to the presence of Pd atoms on the surface. However, only the Pd-based alloys were studied, and other bimetallic compositions could be explored for Hg 0 removal.…”

Section: Introductionmentioning

confidence: 99%

Insights into the Adsorption, Alloy Formation, and Poisoning Effects of Hg on Monometallic and Bimetallic Adsorbents

Mhatre

Bhatia

2022

Langmuir

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The removal of elemental mercury (Hg0) from coal-derived syngas at high temperatures is desired to improve the thermal efficiency of the coal-to-chemical processes. First-principles density functional theory (DFT) calculations for Hg0 adsorption are performed using different exchange correlation functionals (PBE, optPBE-vdW, and optB88-vdW). Gibbs free energy (ΔG) calculations are further performed to evaluate the feasibility of Hg0 adsorption on various exposed planes of metal nanoparticles and to obtain bimetallic compositions for Hg0 removal at various temperatures. Pd and Pt are shown to be suitable for Hg0 adsorption at high temperatures (473 K), whereas Rh and Ru are effective only until 373 K. The bimetallic adsorbents comprising Ag or Au along with Rh, Ru, Pd, or Pt are identified for Hg0 removal at high temperatures (473 K). The increase in Hg0 adsorption strength on various bimetallic surfaces is correlated to the upward shift in the d-band center. Further, calculations predict the tendency of Hg to segregate toward the surface of amalgams and disturb the perfect planar geometry of the Pd, Pt, Rh, Ru, Ir, Cu, Ag, and Au surfaces to form a noncrystalline Hg-rich amalgam surface. An analysis of the binding of various adsorbates (H, O, N, and S) shows that the adsorption becomes significantly weaker on various sites in close proximity to pre-adsorbed Hg. Moreover, for specific combinations of the adsorbate, surface composition, and the site location, the adsorption does not take place on the proximal sites. These results are complemented by the partial density of states calculations, which show changes in the electronic properties of the amalgam surface, thus explaining the poisoning effect of Hg on metallic catalysts.

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“…Many efforts have been carried out to investigate the adsorption and nucleation of transition metals on alumina using first-principles calculations [11]. Wang et al [12] studied the growth of Ir n (n = 1–5) clusters on the dehydrated and hydrated γ-Al 2 O 3 surfaces.…”

Section: Introductionmentioning

confidence: 99%

Interaction of Ethylene with Irn (n = 1–10): From Bare Clusters to γ-Al2O3-Supported Nanoparticles

Shi

Zong

et al. 2019

Nanomaterials

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Comprehending the bond nature of ethylene-metal clusters at the atomic level is important for the design of nanocatalysts and their applications in the fields of fine chemistry and petroleum refining. The growth of Irn (n = 1–10) on γ–Al2O3(110) and ethylene adsorption on bare and γ–Al2O3(110)-supported Irn (n = 1–10) clusters were investigated using the density functional theory (DFT) approach. The mode stability of ethylene adsorption on the bare Irn clusters followed the order π > di-σ > B-T, with the exception of Ir8 where the π structure was less stable than the di-σ configuration. On supported Irn (n = 4–7 and 10) the stability sequence was π > di-σ > di-σ′ (at interface), while on supported Irn (n = 2, 3, 8, and 9) the sequence changed to di-σ > π > di-σ′ (at interface). Two-thirds of ethylene adsorption on the supported Irn clusters were weaker than its adsorption on the bare Irn clusters. The pre-adsorbed ethylene at the interface was found to facilitate the nucleation from the even-sized supported Irn to odd-sized Irn clusters, but hindered the nucleation from the odd-sized Irn to even-sized Irn clusters.

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DFT study of Hg adsorption on M-substituted Pd(1 1 1) and PdM/γ-Al 2 O 3 (1 1 0) (M = Au, Ag, Cu) surfaces

Cited by 13 publications

References 45 publications

Density Functional Theory Investigation into the B and Ga Doped Clean and Water Covered γ-Alumina Surfaces

Density Functional Theory Investigation into the B and Ga Doped Clean and Water Covered γ-Alumina Surfaces

Insights into the Adsorption, Alloy Formation, and Poisoning Effects of Hg on Monometallic and Bimetallic Adsorbents

Interaction of Ethylene with Irn (n = 1–10): From Bare Clusters to γ-Al2O3-Supported Nanoparticles

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