Abstract
Single-site heterogeneous catalysts receive increasing attention due to their unique catalytic properties and well-defined active sites. We report a combined computational and experimental study on a series of silica-supported metal ion hydrogenation catalysts (i.e., In3+, Ga3+, Zn2+, Mn2+, and Ti4+/SiO2). These catalysts were synthesized, characterized, and evaluated for gas-phase propylene hydrogenation. Computational studies were carried out on active-site structures and reaction mechanisms. An activity–descriptor relationship was established, which correlates a computational quantity (reaction free energy of the metal hydride formation) with the experimental reaction rate, as a function of the metal. Microkinetic modeling provided qualitative kinetic insights into the activity–descriptor relationship. This relationship was used to predict the trend of activities in a variety of M/SiO2 catalysts. These fundamental studies and the developed activity–descriptor relationship open up new opportunities for rational design of hydrogenation catalysts.
| Original language | English |
|---|---|
| Pages (from-to) | 73-83 |
| Number of pages | 11 |
| Journal | Polyhedron |
| Volume | 152 |
| DOIs | |
| Publication status | Published - Sep 15 2018 |
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Keywords
- Activity descriptor
- DFT
- Hydrogenation
- Metal ion
- Silica
ASJC Scopus subject areas
- Physical and Theoretical Chemistry
- Inorganic Chemistry
- Materials Chemistry
Cite this
Development of activity–descriptor relationships for supported metal ion hydrogenation catalysts on silica. / Liu, Cong; Camacho-Bunquin, Jeffrey; Ferrandon, Magali; Savara, Aditya; Sohn, Hyuntae; Yang, Dali; Kaphan, David M.; Langeslay, Ryan R.; Ignacio-de Leon, Patricia A.; Liu, Shengsi; Das, Ujjal; Yang, Bing; Hock, Adam S.; Stair, Peter C; Curtiss, Larry A.; Delferro, Massimiliano.
In: Polyhedron, Vol. 152, 15.09.2018, p. 73-83.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Development of activity–descriptor relationships for supported metal ion hydrogenation catalysts on silica
AU - Liu, Cong
AU - Camacho-Bunquin, Jeffrey
AU - Ferrandon, Magali
AU - Savara, Aditya
AU - Sohn, Hyuntae
AU - Yang, Dali
AU - Kaphan, David M.
AU - Langeslay, Ryan R.
AU - Ignacio-de Leon, Patricia A.
AU - Liu, Shengsi
AU - Das, Ujjal
AU - Yang, Bing
AU - Hock, Adam S.
AU - Stair, Peter C
AU - Curtiss, Larry A.
AU - Delferro, Massimiliano
PY - 2018/9/15
Y1 - 2018/9/15
N2 - Single-site heterogeneous catalysts receive increasing attention due to their unique catalytic properties and well-defined active sites. We report a combined computational and experimental study on a series of silica-supported metal ion hydrogenation catalysts (i.e., In3+, Ga3+, Zn2+, Mn2+, and Ti4+/SiO2). These catalysts were synthesized, characterized, and evaluated for gas-phase propylene hydrogenation. Computational studies were carried out on active-site structures and reaction mechanisms. An activity–descriptor relationship was established, which correlates a computational quantity (reaction free energy of the metal hydride formation) with the experimental reaction rate, as a function of the metal. Microkinetic modeling provided qualitative kinetic insights into the activity–descriptor relationship. This relationship was used to predict the trend of activities in a variety of M/SiO2 catalysts. These fundamental studies and the developed activity–descriptor relationship open up new opportunities for rational design of hydrogenation catalysts.
AB - Single-site heterogeneous catalysts receive increasing attention due to their unique catalytic properties and well-defined active sites. We report a combined computational and experimental study on a series of silica-supported metal ion hydrogenation catalysts (i.e., In3+, Ga3+, Zn2+, Mn2+, and Ti4+/SiO2). These catalysts were synthesized, characterized, and evaluated for gas-phase propylene hydrogenation. Computational studies were carried out on active-site structures and reaction mechanisms. An activity–descriptor relationship was established, which correlates a computational quantity (reaction free energy of the metal hydride formation) with the experimental reaction rate, as a function of the metal. Microkinetic modeling provided qualitative kinetic insights into the activity–descriptor relationship. This relationship was used to predict the trend of activities in a variety of M/SiO2 catalysts. These fundamental studies and the developed activity–descriptor relationship open up new opportunities for rational design of hydrogenation catalysts.
KW - Activity descriptor
KW - DFT
KW - Hydrogenation
KW - Metal ion
KW - Silica
UR - http://www.scopus.com/inward/record.url?scp=85049305956&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85049305956&partnerID=8YFLogxK
U2 - 10.1016/j.poly.2018.06.006
DO - 10.1016/j.poly.2018.06.006
M3 - Article
VL - 152
SP - 73
EP - 83
JO - Polyhedron
JF - Polyhedron
SN - 0277-5387
ER -