Development of activity–descriptor relationships for supported metal ion hydrogenation catalysts on silica

Cong Liu, Jeffrey Camacho-Bunquin, Magali Ferrandon, Aditya Savara, Hyuntae Sohn, Dali Yang, David M. Kaphan, Ryan R. Langeslay, Patricia A. Ignacio-de Leon, Shengsi Liu, Ujjal Das, Bing Yang, Adam S. Hock, Peter C Stair, Larry A. Curtiss, Massimiliano Delferro

Research output: Contribution to journalArticle

2 Citations (Scopus)

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 languageEnglish
Pages (from-to)73-83
Number of pages11
JournalPolyhedron
Volume152
DOIs
Publication statusPublished - Sep 15 2018

Fingerprint

Silicon Dioxide
Hydrogenation
hydrogenation
Metal ions
metal ions
Silica
silicon dioxide
catalysts
Catalysts
Metals
metal hydrides
propylene
Hydrides
Free energy
Propylene
Reaction rates
reaction kinetics
Gases
free energy
vapor phases

Keywords

  • Activity descriptor
  • DFT
  • Hydrogenation
  • Metal ion
  • Silica

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Inorganic Chemistry
  • Materials Chemistry

Cite this

Liu, C., Camacho-Bunquin, J., Ferrandon, M., Savara, A., Sohn, H., Yang, D., ... Delferro, M. (2018). Development of activity–descriptor relationships for supported metal ion hydrogenation catalysts on silica. Polyhedron, 152, 73-83. https://doi.org/10.1016/j.poly.2018.06.006

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 journalArticle

Liu, C, Camacho-Bunquin, J, Ferrandon, M, Savara, A, Sohn, H, Yang, D, Kaphan, DM, Langeslay, RR, Ignacio-de Leon, PA, Liu, S, Das, U, Yang, B, Hock, AS, Stair, PC, Curtiss, LA & Delferro, M 2018, 'Development of activity–descriptor relationships for supported metal ion hydrogenation catalysts on silica', Polyhedron, vol. 152, pp. 73-83. https://doi.org/10.1016/j.poly.2018.06.006
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. / Development of activity–descriptor relationships for supported metal ion hydrogenation catalysts on silica. In: Polyhedron. 2018 ; Vol. 152. pp. 73-83.
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