Leveraging molecular metal–support interactions for H2 and N2 activation

Ryan C. Cammarota; Laura J. Clouston; Connie C Lu

doi:10.1016/j.ccr.2016.06.014

Leveraging molecular metal–support interactions for H₂ and N₂ activation

Ryan C. Cammarota, Laura J. Clouston, Connie C Lu

Research output: Contribution to journal › Review article › peer-review

125 Scopus citations

Abstract

Many challenging chemical reactions require precious metal catalysts to proceed. Bio-inspired catalysts featuring multiple earth-abundant metals are an attractive alternative, as they offer boundless possibilities for facilitating processes that the constituent metals cannot mediate on their own. Our work utilizes a supporting metal as an electronic lever for tuning a base metal (Co, Ni) active site via a metal–metal bond. This approach has allowed for the development of metal–support catalysts for reductive N₂ silylation and olefin hydrogenation. The bimetallic catalysts display markedly enhanced activity compared to the analogous single metal centers. In this review, we investigate the role of the supporting metal in substrate binding, activation, and catalysis to inform future efforts in the development and optimization of molecular metal–support catalysts.

Original language	English (US)
Pages (from-to)	100-111
Number of pages	12
Journal	Coordination Chemistry Reviews
Volume	334
DOIs	https://doi.org/10.1016/j.ccr.2016.06.014
State	Published - Mar 1 2017

Bibliographical note

Funding Information:
The authors thank Prof. Laura Gagliardi, Dr. Varinia Bernales, and Dr. Konstantinos D. Vogiatzis for computational insight. The work covered in this review was supported in part by the National Science Foundation (NSF, CHE-1254621) and by the Inorganometallic Catalyst Design Center, an Energy Frontier Research Center funded by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES), under Award DE-SC0012702. L.J.C. was supported by a Doctoral Dissertation Fellowship (University of Minnesota Graduate School).

Publisher Copyright:
© 2016 Elsevier B.V.

Keywords

Bimetallic
Dihydrogen
Dinitrogen
Lewis acid
Metal-metal bonding

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10.1016/j.ccr.2016.06.014

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abstract = "Many challenging chemical reactions require precious metal catalysts to proceed. Bio-inspired catalysts featuring multiple earth-abundant metals are an attractive alternative, as they offer boundless possibilities for facilitating processes that the constituent metals cannot mediate on their own. Our work utilizes a supporting metal as an electronic lever for tuning a base metal (Co, Ni) active site via a metal–metal bond. This approach has allowed for the development of metal–support catalysts for reductive N2 silylation and olefin hydrogenation. The bimetallic catalysts display markedly enhanced activity compared to the analogous single metal centers. In this review, we investigate the role of the supporting metal in substrate binding, activation, and catalysis to inform future efforts in the development and optimization of molecular metal–support catalysts.",

keywords = "Bimetallic, Dihydrogen, Dinitrogen, Lewis acid, Metal-metal bonding",

author = "Cammarota, {Ryan C.} and Clouston, {Laura J.} and Lu, {Connie C}",

note = "Funding Information: The authors thank Prof. Laura Gagliardi, Dr. Varinia Bernales, and Dr. Konstantinos D. Vogiatzis for computational insight. The work covered in this review was supported in part by the National Science Foundation (NSF, CHE-1254621) and by the Inorganometallic Catalyst Design Center, an Energy Frontier Research Center funded by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES), under Award DE-SC0012702. L.J.C. was supported by a Doctoral Dissertation Fellowship (University of Minnesota Graduate School). Publisher Copyright: {\textcopyright} 2016 Elsevier B.V.",

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AU - Lu, Connie C

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N2 - Many challenging chemical reactions require precious metal catalysts to proceed. Bio-inspired catalysts featuring multiple earth-abundant metals are an attractive alternative, as they offer boundless possibilities for facilitating processes that the constituent metals cannot mediate on their own. Our work utilizes a supporting metal as an electronic lever for tuning a base metal (Co, Ni) active site via a metal–metal bond. This approach has allowed for the development of metal–support catalysts for reductive N2 silylation and olefin hydrogenation. The bimetallic catalysts display markedly enhanced activity compared to the analogous single metal centers. In this review, we investigate the role of the supporting metal in substrate binding, activation, and catalysis to inform future efforts in the development and optimization of molecular metal–support catalysts.

AB - Many challenging chemical reactions require precious metal catalysts to proceed. Bio-inspired catalysts featuring multiple earth-abundant metals are an attractive alternative, as they offer boundless possibilities for facilitating processes that the constituent metals cannot mediate on their own. Our work utilizes a supporting metal as an electronic lever for tuning a base metal (Co, Ni) active site via a metal–metal bond. This approach has allowed for the development of metal–support catalysts for reductive N2 silylation and olefin hydrogenation. The bimetallic catalysts display markedly enhanced activity compared to the analogous single metal centers. In this review, we investigate the role of the supporting metal in substrate binding, activation, and catalysis to inform future efforts in the development and optimization of molecular metal–support catalysts.

KW - Bimetallic

KW - Dihydrogen

KW - Dinitrogen

KW - Lewis acid

KW - Metal-metal bonding

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JO - Coordination Chemistry Reviews

JF - Coordination Chemistry Reviews

ER -

Leveraging molecular metal–support interactions for H₂ and N₂ activation

Abstract

Bibliographical note

Keywords

Publisher link

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Energy Frontier Research Center For Inorganometallic Catalyst Design (DE-SC0012702)

Cite this

Leveraging molecular metal–support interactions for H2 and N2 activation

Abstract

Bibliographical note

Keywords

Publisher link

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Projects

Energy Frontier Research Center For Inorganometallic Catalyst Design (DE-SC0012702)

Cite this

Leveraging molecular metal–support interactions for H₂ and N₂ activation