Rhodium catechol containing porous organic polymers: Defined catalysis for single-site and supported nanoparticulate materials

Steven J. Kraft; Guanghui Zhang; David Childers; Fulya Dogan; Jeffrey T. Miller; Sonbinh T. Nguyen; Adam S. Hock

doi:10.1021/om500136k

Rhodium catechol containing porous organic polymers: Defined catalysis for single-site and supported nanoparticulate materials

Steven J. Kraft, Guanghui Zhang, David Childers, Fulya Dogan, Jeffrey T. Miller, Sonbinh T. Nguyen, Adam S. Hock^*

^*Corresponding author for this work

Chemistry

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

21 Scopus citations

Abstract

A single-site, rhodium(I) catecholate containing porous organic polymer was prepared and utilized as an active catalyst for the hydrogenation of olefins in both liquid-phase and gas-phase reactors. Liquid-phase, batch hydrogenation reactions at 50 psi and ambient temperatures result in the formation of rhodium metal nanoparticles supported within the polymer framework. Surprisingly, the Rh(I) complex is catalytically active and stable for propene hydrogenation at ambient temperatures under gas-phase conditions, where reduction of the Rh(I) centers to Rh(0) nanoparticles requires at least 200-250 °C under a flow of hydrogen gas. After high-temperature treatment, the Rh(0) nanoparticles are active arene hydrogenation catalysts that convert toluene to methylcyclohexadiene at a rate of 9.3 × 10^-3 mol g^-1 h^-1 of rhodium metal at room temperature. Conversely, single-site Rh(I) is an active and stable catalyst for the hydrogenation of propylene (but not toluene) under gas-phase conditions at room temperature.

Original language	English (US)
Pages (from-to)	2517-2522
Number of pages	6
Journal	Organometallics
Volume	33
Issue number	10
DOIs	https://doi.org/10.1021/om500136k
State	Published - May 27 2014

ASJC Scopus subject areas

Physical and Theoretical Chemistry
Organic Chemistry
Inorganic Chemistry

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@article{173126ac9b2c43e981fc0c4fba9f9411,

title = "Rhodium catechol containing porous organic polymers: Defined catalysis for single-site and supported nanoparticulate materials",

abstract = "A single-site, rhodium(I) catecholate containing porous organic polymer was prepared and utilized as an active catalyst for the hydrogenation of olefins in both liquid-phase and gas-phase reactors. Liquid-phase, batch hydrogenation reactions at 50 psi and ambient temperatures result in the formation of rhodium metal nanoparticles supported within the polymer framework. Surprisingly, the Rh(I) complex is catalytically active and stable for propene hydrogenation at ambient temperatures under gas-phase conditions, where reduction of the Rh(I) centers to Rh(0) nanoparticles requires at least 200-250 °C under a flow of hydrogen gas. After high-temperature treatment, the Rh(0) nanoparticles are active arene hydrogenation catalysts that convert toluene to methylcyclohexadiene at a rate of 9.3 × 10-3 mol g-1 h-1 of rhodium metal at room temperature. Conversely, single-site Rh(I) is an active and stable catalyst for the hydrogenation of propylene (but not toluene) under gas-phase conditions at room temperature.",

author = "Kraft, {Steven J.} and Guanghui Zhang and David Childers and Fulya Dogan and Miller, {Jeffrey T.} and Nguyen, {Sonbinh T.} and Hock, {Adam S.}",

year = "2014",

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doi = "10.1021/om500136k",

language = "English (US)",

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T1 - Rhodium catechol containing porous organic polymers

T2 - Defined catalysis for single-site and supported nanoparticulate materials

AU - Kraft, Steven J.

AU - Zhang, Guanghui

AU - Childers, David

AU - Dogan, Fulya

AU - Miller, Jeffrey T.

AU - Nguyen, Sonbinh T.

AU - Hock, Adam S.

PY - 2014/5/27

Y1 - 2014/5/27

N2 - A single-site, rhodium(I) catecholate containing porous organic polymer was prepared and utilized as an active catalyst for the hydrogenation of olefins in both liquid-phase and gas-phase reactors. Liquid-phase, batch hydrogenation reactions at 50 psi and ambient temperatures result in the formation of rhodium metal nanoparticles supported within the polymer framework. Surprisingly, the Rh(I) complex is catalytically active and stable for propene hydrogenation at ambient temperatures under gas-phase conditions, where reduction of the Rh(I) centers to Rh(0) nanoparticles requires at least 200-250 °C under a flow of hydrogen gas. After high-temperature treatment, the Rh(0) nanoparticles are active arene hydrogenation catalysts that convert toluene to methylcyclohexadiene at a rate of 9.3 × 10-3 mol g-1 h-1 of rhodium metal at room temperature. Conversely, single-site Rh(I) is an active and stable catalyst for the hydrogenation of propylene (but not toluene) under gas-phase conditions at room temperature.

AB - A single-site, rhodium(I) catecholate containing porous organic polymer was prepared and utilized as an active catalyst for the hydrogenation of olefins in both liquid-phase and gas-phase reactors. Liquid-phase, batch hydrogenation reactions at 50 psi and ambient temperatures result in the formation of rhodium metal nanoparticles supported within the polymer framework. Surprisingly, the Rh(I) complex is catalytically active and stable for propene hydrogenation at ambient temperatures under gas-phase conditions, where reduction of the Rh(I) centers to Rh(0) nanoparticles requires at least 200-250 °C under a flow of hydrogen gas. After high-temperature treatment, the Rh(0) nanoparticles are active arene hydrogenation catalysts that convert toluene to methylcyclohexadiene at a rate of 9.3 × 10-3 mol g-1 h-1 of rhodium metal at room temperature. Conversely, single-site Rh(I) is an active and stable catalyst for the hydrogenation of propylene (but not toluene) under gas-phase conditions at room temperature.

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JO - Organometallics

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IS - 10

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Rhodium catechol containing porous organic polymers: Defined catalysis for single-site and supported nanoparticulate materials

Abstract

ASJC Scopus subject areas

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