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

doi:10.1016/j.poly.2018.06.006

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

Northwestern University

Research output: Contribution to journal › Article › peer-review

3 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 language	English
Pages (from-to)	73-83
Number of pages	11
Journal	Polyhedron
Volume	152
DOIs	https://doi.org/10.1016/j.poly.2018.06.006
Publication status	Published - Sep 15 2018

Keywords

Activity descriptor
DFT
Hydrogenation
Metal ion
Silica

ASJC Scopus subject areas

Physical and Theoretical Chemistry
Inorganic Chemistry
Materials Chemistry

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Liu, C., Camacho-Bunquin, J., Ferrandon, M., Savara, A., Sohn, H., Yang, D., Kaphan, D. M., Langeslay, R. R., Ignacio-de Leon, P. A., Liu, S., Das, U., Yang, B., Hock, A. S., Stair, P. C., Curtiss, L. A., & 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 journal › Article › peer-review

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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title = "Development of activity–descriptor relationships for supported metal ion hydrogenation catalysts on silica",

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.",

keywords = "Activity descriptor, DFT, Hydrogenation, Metal ion, Silica",

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

note = "Funding Information: This work was supported by the U.S. Department of Energy (DOE), Office of Basic Energy Sciences , Division of Chemical Sciences, Geosciences, and Biosciences, under Contract DE-AC02-06CH11357 ( Argonne National Laboratory ). DFT calculations were performed using the computational resources at the Argonne National Laboratory (ANL), Center for Nanoscale Materials (CNM) and resources provided by the Laboratory Computing Resource Center (LCRC) at ANL. Use of the Advanced Photon Source is supported by the U.S. Department of Energy, Office of Science, and Office of the Basic Energy Sciences, under Contract DE-AC-02-06CH11357. MRCAT operations are supported by the Department of Energy and the MRCAT member institutions. Microkinetic modeling was supported by the U.S. Department of Energy (DOE), Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences, under Contract DE-AC05-00OR22725 (ORNL). The XPS work made use of the facilities of the NU ANCE Center at Northwestern University, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource ( NSF NNCI-1542205 ); the MRSEC Program (NSF DMR-1121262 ) at the Materials Research Center ; the International Institute for Nanotechnology ( IIN ); the Keck Foundation ; and the State of Illinois, through the IIN. ",

year = "2018",

month = sep,

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doi = "10.1016/j.poly.2018.06.006",

language = "English",

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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

N1 - Funding Information: This work was supported by the U.S. Department of Energy (DOE), Office of Basic Energy Sciences , Division of Chemical Sciences, Geosciences, and Biosciences, under Contract DE-AC02-06CH11357 ( Argonne National Laboratory ). DFT calculations were performed using the computational resources at the Argonne National Laboratory (ANL), Center for Nanoscale Materials (CNM) and resources provided by the Laboratory Computing Resource Center (LCRC) at ANL. Use of the Advanced Photon Source is supported by the U.S. Department of Energy, Office of Science, and Office of the Basic Energy Sciences, under Contract DE-AC-02-06CH11357. MRCAT operations are supported by the Department of Energy and the MRCAT member institutions. Microkinetic modeling was supported by the U.S. Department of Energy (DOE), Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences, under Contract DE-AC05-00OR22725 (ORNL). The XPS work made use of the facilities of the NU ANCE Center at Northwestern University, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource ( NSF NNCI-1542205 ); the MRSEC Program (NSF DMR-1121262 ) at the Materials Research Center ; the International Institute for Nanotechnology ( IIN ); the Keck Foundation ; and the State of Illinois, through the IIN.

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.

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KW - Metal ion

KW - Silica

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