Abstract
Spin-polarized density functional theory studies of hydrogen sulfide (H2S) adsorption and decomposition on Ni(100) and Ni 3Al(100) surfaces were conducted to understand the aluminum (Al) alloying effect on H2S dissociation. For such purpose, we first determined the near surface structure of fully ordered Ni3Al alloy along the [100] direction by calculating the Al segregation energy to the surface and then examined the adsorption energies of the adsorbates (H 2S, HS, S, and H) and the activation barriers for the H2S and HS decomposition by using Climbing Image-Nudged Elastic Band method. We found that regardless of the way to terminate the surface, Al atom in bimetallic Ni3Al(100) tends to exist in the first surface layer, rather than in the second or third layer, and the Ni3Al(100) surface can substantially retard the H2S decomposition by reducing the adsorption energy of sulfur compounds compared to the pure Ni(100) case. Finally, we presented how the Al in Ni3Al modifies the activity of surface Ni atoms toward the sulfur compounds by calculating the local density of states and charge distribution in alloying components. This work hints the importance of knowing how to properly tailor the reactivity of Ni based materials to enhance the resistance for sulfur poisoning.
| Original language | English |
|---|---|
| Pages (from-to) | 12251-12258 |
| Number of pages | 8 |
| Journal | International Journal of Hydrogen Energy |
| Volume | 39 |
| Issue number | 23 |
| DOIs | |
| Publication status | Published - 2014 Aug 4 |
| Externally published | Yes |
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ASJC Scopus subject areas
- Renewable Energy, Sustainability and the Environment
- Fuel Technology
- Condensed Matter Physics
- Energy Engineering and Power Technology
Cite this
Decomposition of hydrogen sulfide (H2S) on Ni(100) and Ni 3Al(100) surfaces from first-principles. / Hernandez, Juan Martin; Lim, Dong Hee; Nguyen, Hoang Viet Phuc; Yoon, Sung Pil; Han, Jonghee; Nam, SukWoo; Yoon, Chang Won; Kim, Soo Kil; Ham, Hyung Chul.
In: International Journal of Hydrogen Energy, Vol. 39, No. 23, 04.08.2014, p. 12251-12258.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Decomposition of hydrogen sulfide (H2S) on Ni(100) and Ni 3Al(100) surfaces from first-principles
AU - Hernandez, Juan Martin
AU - Lim, Dong Hee
AU - Nguyen, Hoang Viet Phuc
AU - Yoon, Sung Pil
AU - Han, Jonghee
AU - Nam, SukWoo
AU - Yoon, Chang Won
AU - Kim, Soo Kil
AU - Ham, Hyung Chul
PY - 2014/8/4
Y1 - 2014/8/4
N2 - Spin-polarized density functional theory studies of hydrogen sulfide (H2S) adsorption and decomposition on Ni(100) and Ni 3Al(100) surfaces were conducted to understand the aluminum (Al) alloying effect on H2S dissociation. For such purpose, we first determined the near surface structure of fully ordered Ni3Al alloy along the [100] direction by calculating the Al segregation energy to the surface and then examined the adsorption energies of the adsorbates (H 2S, HS, S, and H) and the activation barriers for the H2S and HS decomposition by using Climbing Image-Nudged Elastic Band method. We found that regardless of the way to terminate the surface, Al atom in bimetallic Ni3Al(100) tends to exist in the first surface layer, rather than in the second or third layer, and the Ni3Al(100) surface can substantially retard the H2S decomposition by reducing the adsorption energy of sulfur compounds compared to the pure Ni(100) case. Finally, we presented how the Al in Ni3Al modifies the activity of surface Ni atoms toward the sulfur compounds by calculating the local density of states and charge distribution in alloying components. This work hints the importance of knowing how to properly tailor the reactivity of Ni based materials to enhance the resistance for sulfur poisoning.
AB - Spin-polarized density functional theory studies of hydrogen sulfide (H2S) adsorption and decomposition on Ni(100) and Ni 3Al(100) surfaces were conducted to understand the aluminum (Al) alloying effect on H2S dissociation. For such purpose, we first determined the near surface structure of fully ordered Ni3Al alloy along the [100] direction by calculating the Al segregation energy to the surface and then examined the adsorption energies of the adsorbates (H 2S, HS, S, and H) and the activation barriers for the H2S and HS decomposition by using Climbing Image-Nudged Elastic Band method. We found that regardless of the way to terminate the surface, Al atom in bimetallic Ni3Al(100) tends to exist in the first surface layer, rather than in the second or third layer, and the Ni3Al(100) surface can substantially retard the H2S decomposition by reducing the adsorption energy of sulfur compounds compared to the pure Ni(100) case. Finally, we presented how the Al in Ni3Al modifies the activity of surface Ni atoms toward the sulfur compounds by calculating the local density of states and charge distribution in alloying components. This work hints the importance of knowing how to properly tailor the reactivity of Ni based materials to enhance the resistance for sulfur poisoning.
KW - (100) facet
KW - Density functional theory
KW - Ligand
UR - http://www.scopus.com/inward/record.url?scp=84904739964&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=84904739964&partnerID=8YFLogxK
U2 - 10.1016/j.ijhydene.2014.03.064
DO - 10.1016/j.ijhydene.2014.03.064
M3 - Article
VL - 39
SP - 12251
EP - 12258
JO - International Journal of Hydrogen Energy
JF - International Journal of Hydrogen Energy
SN - 0360-3199
IS - 23
ER -