Dynamic equilibria in supported ionic liquid phase (SILP) catalysis: in situ IR spectroscopy identifies [Ru(CO) x Cl y ] n species in water gas shift catalysis
Ru-based supported ionic liquid phase (SILP) systems efficiently catalyze the low-temperature water-gas shift reaction (WGSR). While previous studies suggest that Ru-carbonyl species play an important role in the mechanism, detailed knowledge on the catalytically active species is still missing. To...
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| Veröffentlicht in: | Catalysis science & technology 2018, Vol.8 (1), p.344-357 |
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| creator | Bauer, Tanja Stepic, Robert Wolf, Patrick Kollhoff, Fabian Karawacka, Weronika Wick, Christian R. Haumann, Marco Wasserscheid, Peter Smith, David M. Smith, Ana-Sunčana Libuda, Jörg |
| description | Ru-based supported ionic liquid phase (SILP) systems efficiently catalyze the low-temperature water-gas shift reaction (WGSR). While previous studies suggest that Ru-carbonyl species play an important role in the mechanism, detailed knowledge on the catalytically active species is still missing. To identify these carbonyl complexes, we apply
in situ
diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) in combination with density functional theory (DFT). Investigations of an as-prepared [Ru(CO)
3
Cl
2
]
2
/[C
4
C
1
C
1
Im]Cl/Al
2
O
3
catalyst indicate splitting of the dimer induced by Cl
−
. Subsequently, an equilibrium between several [Ru(CO)
x
Cl
y
]
n
species is established, in which the IL serves as an effectively infinite Cl
−
reservoir. We find that the major species in the system freshly-prepared from [Ru(CO)
3
Cl
2
]
2
is indeed [Ru(CO)
3
Cl
3
]
−
. A smaller amount of [Ru(CO)
2
Cl
3
]
−
and chloride-rich species [Ru(CO)
2
Cl
4
]
2−
or [RuCOCl
4
]
2−
are also found in the SILP. Similar Ru-carbonyl species are observed during carbonylation of RuCl
3
/[C
4
C
1
C
1
Im]Cl/Al
2
O
3
, another potential WGSR catalyst. The response of [Ru(CO)
3
Cl
2
]
2
/[C
4
C
1
C
1
Im]Cl/Al
2
O
3
to heating and/or CO dosing was probed
in situ
and the results confirm the presence of the equilibrium proposed above. |
| doi_str_mv | 10.1039/C7CY02199B |
| format | Article |
| fullrecord | <record><control><sourceid>proquest_cross</sourceid><recordid>TN_cdi_proquest_journals_2010867343</recordid><sourceformat>XML</sourceformat><sourcesystem>PC</sourcesystem><sourcerecordid>2010867343</sourcerecordid><originalsourceid>FETCH-LOGICAL-c247b-9d4bb2c1d39d79ac2db9134538d8fb80e282e19477c3c1665e987cd129a4fd173</originalsourceid><addsrcrecordid>eNpFUdtKw0AQDaJgqX3xCwZ8aYXq3trN-qbxVihUqj6ISNjsbuyWNEl3EzRf46-atmLnZQbOZZg5QXCK0QVGVFxGPHpDBAtxcxB0CGJsyPgYH_7PI3oc9LxforaYwCgkneDntsnlyiow69pmNnFWgs3B12VZuMposEXeopltYQ3lQnoD_efJ9GkASlYya7z1V1uFrWqYzMGXRlWu8KooG7Da5JVNrfHwPq_70WwA3xBl0MAH5FvqBmrVX7IyDj6lB7-wabX3PgmOUpl50_vr3eD1_u4lehxOZw-T6Ho6VITxZCg0SxKisKZCcyEV0YnAlI1oqMM0CZEhITFYMM4VVXg8HhkRcqUxEZKlGnPaDc52vqUr1rXxVbwsape3K2OC2leNOWW0ZZ3vWKq90DuTxqWzK-maGKN4k0G8z4D-AoYveVQ</addsrcrecordid><sourcetype>Aggregation Database</sourcetype><iscdi>true</iscdi><recordtype>article</recordtype><pqid>2010867343</pqid></control><display><type>article</type><title>Dynamic equilibria in supported ionic liquid phase (SILP) catalysis: in situ IR spectroscopy identifies [Ru(CO) x Cl y ] n species in water gas shift catalysis</title><source>Royal Society Of Chemistry Journals 2008-</source><creator>Bauer, Tanja ; Stepic, Robert ; Wolf, Patrick ; Kollhoff, Fabian ; Karawacka, Weronika ; Wick, Christian R. ; Haumann, Marco ; Wasserscheid, Peter ; Smith, David M. ; Smith, Ana-Sunčana ; Libuda, Jörg</creator><creatorcontrib>Bauer, Tanja ; Stepic, Robert ; Wolf, Patrick ; Kollhoff, Fabian ; Karawacka, Weronika ; Wick, Christian R. ; Haumann, Marco ; Wasserscheid, Peter ; Smith, David M. ; Smith, Ana-Sunčana ; Libuda, Jörg</creatorcontrib><description>Ru-based supported ionic liquid phase (SILP) systems efficiently catalyze the low-temperature water-gas shift reaction (WGSR). While previous studies suggest that Ru-carbonyl species play an important role in the mechanism, detailed knowledge on the catalytically active species is still missing. To identify these carbonyl complexes, we apply
in situ
diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) in combination with density functional theory (DFT). Investigations of an as-prepared [Ru(CO)
3
Cl
2
]
2
/[C
4
C
1
C
1
Im]Cl/Al
2
O
3
catalyst indicate splitting of the dimer induced by Cl
−
. Subsequently, an equilibrium between several [Ru(CO)
x
Cl
y
]
n
species is established, in which the IL serves as an effectively infinite Cl
−
reservoir. We find that the major species in the system freshly-prepared from [Ru(CO)
3
Cl
2
]
2
is indeed [Ru(CO)
3
Cl
3
]
−
. A smaller amount of [Ru(CO)
2
Cl
3
]
−
and chloride-rich species [Ru(CO)
2
Cl
4
]
2−
or [RuCOCl
4
]
2−
are also found in the SILP. Similar Ru-carbonyl species are observed during carbonylation of RuCl
3
/[C
4
C
1
C
1
Im]Cl/Al
2
O
3
, another potential WGSR catalyst. The response of [Ru(CO)
3
Cl
2
]
2
/[C
4
C
1
C
1
Im]Cl/Al
2
O
3
to heating and/or CO dosing was probed
in situ
and the results confirm the presence of the equilibrium proposed above.</description><identifier>ISSN: 2044-4753</identifier><identifier>EISSN: 2044-4761</identifier><identifier>DOI: 10.1039/C7CY02199B</identifier><language>eng</language><publisher>Cambridge: Royal Society of Chemistry</publisher><subject>Aluminum oxide ; Carbonyls ; Catalysis ; Catalysts ; Density functional theory ; Diffuse reflectance spectroscopy ; Fourier transforms ; Infrared spectroscopy ; Ionic liquids ; Ions ; Ruthenium trichloride ; Shift reaction ; Spectrum analysis ; Water gas</subject><ispartof>Catalysis science & technology, 2018, Vol.8 (1), p.344-357</ispartof><rights>Copyright Royal Society of Chemistry 2018</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c247b-9d4bb2c1d39d79ac2db9134538d8fb80e282e19477c3c1665e987cd129a4fd173</citedby><cites>FETCH-LOGICAL-c247b-9d4bb2c1d39d79ac2db9134538d8fb80e282e19477c3c1665e987cd129a4fd173</cites><orcidid>0000-0002-3896-365X ; 0000-0002-6399-2954</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>315,781,785,4025,27928,27929,27930</link.rule.ids></links><search><creatorcontrib>Bauer, Tanja</creatorcontrib><creatorcontrib>Stepic, Robert</creatorcontrib><creatorcontrib>Wolf, Patrick</creatorcontrib><creatorcontrib>Kollhoff, Fabian</creatorcontrib><creatorcontrib>Karawacka, Weronika</creatorcontrib><creatorcontrib>Wick, Christian R.</creatorcontrib><creatorcontrib>Haumann, Marco</creatorcontrib><creatorcontrib>Wasserscheid, Peter</creatorcontrib><creatorcontrib>Smith, David M.</creatorcontrib><creatorcontrib>Smith, Ana-Sunčana</creatorcontrib><creatorcontrib>Libuda, Jörg</creatorcontrib><title>Dynamic equilibria in supported ionic liquid phase (SILP) catalysis: in situ IR spectroscopy identifies [Ru(CO) x Cl y ] n species in water gas shift catalysis</title><title>Catalysis science & technology</title><description>Ru-based supported ionic liquid phase (SILP) systems efficiently catalyze the low-temperature water-gas shift reaction (WGSR). While previous studies suggest that Ru-carbonyl species play an important role in the mechanism, detailed knowledge on the catalytically active species is still missing. To identify these carbonyl complexes, we apply
in situ
diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) in combination with density functional theory (DFT). Investigations of an as-prepared [Ru(CO)
3
Cl
2
]
2
/[C
4
C
1
C
1
Im]Cl/Al
2
O
3
catalyst indicate splitting of the dimer induced by Cl
−
. Subsequently, an equilibrium between several [Ru(CO)
x
Cl
y
]
n
species is established, in which the IL serves as an effectively infinite Cl
−
reservoir. We find that the major species in the system freshly-prepared from [Ru(CO)
3
Cl
2
]
2
is indeed [Ru(CO)
3
Cl
3
]
−
. A smaller amount of [Ru(CO)
2
Cl
3
]
−
and chloride-rich species [Ru(CO)
2
Cl
4
]
2−
or [RuCOCl
4
]
2−
are also found in the SILP. Similar Ru-carbonyl species are observed during carbonylation of RuCl
3
/[C
4
C
1
C
1
Im]Cl/Al
2
O
3
, another potential WGSR catalyst. The response of [Ru(CO)
3
Cl
2
]
2
/[C
4
C
1
C
1
Im]Cl/Al
2
O
3
to heating and/or CO dosing was probed
in situ
and the results confirm the presence of the equilibrium proposed above.</description><subject>Aluminum oxide</subject><subject>Carbonyls</subject><subject>Catalysis</subject><subject>Catalysts</subject><subject>Density functional theory</subject><subject>Diffuse reflectance spectroscopy</subject><subject>Fourier transforms</subject><subject>Infrared spectroscopy</subject><subject>Ionic liquids</subject><subject>Ions</subject><subject>Ruthenium trichloride</subject><subject>Shift reaction</subject><subject>Spectrum analysis</subject><subject>Water gas</subject><issn>2044-4753</issn><issn>2044-4761</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2018</creationdate><recordtype>article</recordtype><recordid>eNpFUdtKw0AQDaJgqX3xCwZ8aYXq3trN-qbxVihUqj6ISNjsbuyWNEl3EzRf46-atmLnZQbOZZg5QXCK0QVGVFxGPHpDBAtxcxB0CGJsyPgYH_7PI3oc9LxforaYwCgkneDntsnlyiow69pmNnFWgs3B12VZuMposEXeopltYQ3lQnoD_efJ9GkASlYya7z1V1uFrWqYzMGXRlWu8KooG7Da5JVNrfHwPq_70WwA3xBl0MAH5FvqBmrVX7IyDj6lB7-wabX3PgmOUpl50_vr3eD1_u4lehxOZw-T6Ho6VITxZCg0SxKisKZCcyEV0YnAlI1oqMM0CZEhITFYMM4VVXg8HhkRcqUxEZKlGnPaDc52vqUr1rXxVbwsape3K2OC2leNOWW0ZZ3vWKq90DuTxqWzK-maGKN4k0G8z4D-AoYveVQ</recordid><startdate>2018</startdate><enddate>2018</enddate><creator>Bauer, Tanja</creator><creator>Stepic, Robert</creator><creator>Wolf, Patrick</creator><creator>Kollhoff, Fabian</creator><creator>Karawacka, Weronika</creator><creator>Wick, Christian R.</creator><creator>Haumann, Marco</creator><creator>Wasserscheid, Peter</creator><creator>Smith, David M.</creator><creator>Smith, Ana-Sunčana</creator><creator>Libuda, Jörg</creator><general>Royal Society of Chemistry</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7SR</scope><scope>8BQ</scope><scope>8FD</scope><scope>JG9</scope><orcidid>https://orcid.org/0000-0002-3896-365X</orcidid><orcidid>https://orcid.org/0000-0002-6399-2954</orcidid></search><sort><creationdate>2018</creationdate><title>Dynamic equilibria in supported ionic liquid phase (SILP) catalysis: in situ IR spectroscopy identifies [Ru(CO) x Cl y ] n species in water gas shift catalysis</title><author>Bauer, Tanja ; Stepic, Robert ; Wolf, Patrick ; Kollhoff, Fabian ; Karawacka, Weronika ; Wick, Christian R. ; Haumann, Marco ; Wasserscheid, Peter ; Smith, David M. ; Smith, Ana-Sunčana ; Libuda, Jörg</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c247b-9d4bb2c1d39d79ac2db9134538d8fb80e282e19477c3c1665e987cd129a4fd173</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2018</creationdate><topic>Aluminum oxide</topic><topic>Carbonyls</topic><topic>Catalysis</topic><topic>Catalysts</topic><topic>Density functional theory</topic><topic>Diffuse reflectance spectroscopy</topic><topic>Fourier transforms</topic><topic>Infrared spectroscopy</topic><topic>Ionic liquids</topic><topic>Ions</topic><topic>Ruthenium trichloride</topic><topic>Shift reaction</topic><topic>Spectrum analysis</topic><topic>Water gas</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Bauer, Tanja</creatorcontrib><creatorcontrib>Stepic, Robert</creatorcontrib><creatorcontrib>Wolf, Patrick</creatorcontrib><creatorcontrib>Kollhoff, Fabian</creatorcontrib><creatorcontrib>Karawacka, Weronika</creatorcontrib><creatorcontrib>Wick, Christian R.</creatorcontrib><creatorcontrib>Haumann, Marco</creatorcontrib><creatorcontrib>Wasserscheid, Peter</creatorcontrib><creatorcontrib>Smith, David M.</creatorcontrib><creatorcontrib>Smith, Ana-Sunčana</creatorcontrib><creatorcontrib>Libuda, Jörg</creatorcontrib><collection>CrossRef</collection><collection>Engineered Materials Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Materials Research Database</collection><jtitle>Catalysis science & technology</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Bauer, Tanja</au><au>Stepic, Robert</au><au>Wolf, Patrick</au><au>Kollhoff, Fabian</au><au>Karawacka, Weronika</au><au>Wick, Christian R.</au><au>Haumann, Marco</au><au>Wasserscheid, Peter</au><au>Smith, David M.</au><au>Smith, Ana-Sunčana</au><au>Libuda, Jörg</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Dynamic equilibria in supported ionic liquid phase (SILP) catalysis: in situ IR spectroscopy identifies [Ru(CO) x Cl y ] n species in water gas shift catalysis</atitle><jtitle>Catalysis science & technology</jtitle><date>2018</date><risdate>2018</risdate><volume>8</volume><issue>1</issue><spage>344</spage><epage>357</epage><pages>344-357</pages><issn>2044-4753</issn><eissn>2044-4761</eissn><abstract>Ru-based supported ionic liquid phase (SILP) systems efficiently catalyze the low-temperature water-gas shift reaction (WGSR). While previous studies suggest that Ru-carbonyl species play an important role in the mechanism, detailed knowledge on the catalytically active species is still missing. To identify these carbonyl complexes, we apply
in situ
diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) in combination with density functional theory (DFT). Investigations of an as-prepared [Ru(CO)
3
Cl
2
]
2
/[C
4
C
1
C
1
Im]Cl/Al
2
O
3
catalyst indicate splitting of the dimer induced by Cl
−
. Subsequently, an equilibrium between several [Ru(CO)
x
Cl
y
]
n
species is established, in which the IL serves as an effectively infinite Cl
−
reservoir. We find that the major species in the system freshly-prepared from [Ru(CO)
3
Cl
2
]
2
is indeed [Ru(CO)
3
Cl
3
]
−
. A smaller amount of [Ru(CO)
2
Cl
3
]
−
and chloride-rich species [Ru(CO)
2
Cl
4
]
2−
or [RuCOCl
4
]
2−
are also found in the SILP. Similar Ru-carbonyl species are observed during carbonylation of RuCl
3
/[C
4
C
1
C
1
Im]Cl/Al
2
O
3
, another potential WGSR catalyst. The response of [Ru(CO)
3
Cl
2
]
2
/[C
4
C
1
C
1
Im]Cl/Al
2
O
3
to heating and/or CO dosing was probed
in situ
and the results confirm the presence of the equilibrium proposed above.</abstract><cop>Cambridge</cop><pub>Royal Society of Chemistry</pub><doi>10.1039/C7CY02199B</doi><tpages>14</tpages><orcidid>https://orcid.org/0000-0002-3896-365X</orcidid><orcidid>https://orcid.org/0000-0002-6399-2954</orcidid><oa>free_for_read</oa></addata></record> |
| fulltext | fulltext |
| identifier | ISSN: 2044-4753 |
| ispartof | Catalysis science & technology, 2018, Vol.8 (1), p.344-357 |
| issn | 2044-4753 2044-4761 |
| language | eng |
| recordid | cdi_proquest_journals_2010867343 |
| source | Royal Society Of Chemistry Journals 2008- |
| subjects | Aluminum oxide Carbonyls Catalysis Catalysts Density functional theory Diffuse reflectance spectroscopy Fourier transforms Infrared spectroscopy Ionic liquids Ions Ruthenium trichloride Shift reaction Spectrum analysis Water gas |
| title | Dynamic equilibria in supported ionic liquid phase (SILP) catalysis: in situ IR spectroscopy identifies [Ru(CO) x Cl y ] n species in water gas shift catalysis |
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