Catalytic Activity of Molecular Rhenium Sulfide Clusters [Re6S8(OH)6−n(H2O)n](4−n)− (n = 0, 2, 4, 6) with Retention of the Octahedral Metal Frameworks: Dehydrogenation and Dehydration of 1,4-Butanediol
A series of molecular rhenium sulfide clusters [Re 6 S 8 (OH) 6− n (H 2 O) n ] (4− n )− ( n = 0, 2, 4, 6) catalyze dehydrogenation of alcohols, and hydrogenation of ketones and olefins in a hydrogen stream at 350 °C. The catalytic activities of the dianionic and neutral clusters ( n = 2, 4) are lo...
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| Veröffentlicht in: | Journal of cluster science 2014-09, Vol.25 (5), p.1203-1224 |
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| creator | Nagashima, Sayoko Furukawa, Shota Kamiguchi, Satoshi Kajio, Ryu Nagashima, Hiroshi Yamaguchi, Aritomo Shirai, Masayuki Kurokawa, Hideki Chihara, Teiji |
| description | A series of molecular rhenium sulfide clusters [Re
6
S
8
(OH)
6−
n
(H
2
O)
n
]
(4−
n
)−
(
n
= 0, 2, 4, 6) catalyze dehydrogenation of alcohols, and hydrogenation of ketones and olefins in a hydrogen stream at 350 °C. The catalytic activities of the dianionic and neutral clusters (
n
= 2, 4) are lower than those of tetraanionic and dicationic clusters (
n
= 0, 6) for all the reactions. When 1,4-butanediol is allowed to react over K
4
[Re
6
S
8
(OH)
6
], dehydrogenation proceeds to yield 2-hydroxytetrahydrofuran and successively γ-butyrolactone above 300 °C. Over [Re
6
S
8
(H
2
O)
6
]SO
4
dehydration proceeds to yield tetrahydrofuran above 250 °C. The thermal activation mechanisms of these clusters were studied by powder X-ray diffraction analyses, Raman spectrometry, extended X-ray absorption fine structure spectrometry, thermogravimetry, and differential thermal analyses. The catalytically active site of K
4
[Re
6
S
8
(OH)
6
] is an uncoordinated metal site (Lewis acid site) developed by the loss of a water molecule from two hydroxo ligands. The active site of [Re
6
S
8
(H
2
O)
6
]SO
4
is a Brønsted acid site; the anhydrous aqua cluster dication disproportionates to a hydroxo cluster monocation and a proton. Both of the octahedral cluster frameworks are retained up to 500 °C. |
| doi_str_mv | 10.1007/s10876-014-0700-x |
| format | Article |
| fullrecord | <record><control><sourceid>proquest_cross</sourceid><recordid>TN_cdi_proquest_journals_2918277495</recordid><sourceformat>XML</sourceformat><sourcesystem>PC</sourcesystem><sourcerecordid>2918277495</sourcerecordid><originalsourceid>FETCH-LOGICAL-c386t-32449e237ff4e3f9bd0dc4e42adf4b91373ed1ca0dd58a0d76ef1d3d941901103</originalsourceid><addsrcrecordid>eNp1UU1uEzEUHiGQKIUDsLPEJpEy5fknYw8Si5K2BKlVpBRWCFnu-E1nysQutqdtbsCaE_QsvQFX4CRMSFFX3bw_fT9P-rLsNYU9CiDfRgpKFjlQkYMEyG-eZDt0KlmuVMGeDjMIyCWT6nn2IsYLACgV5zvZ75lJpluntiL7VWqv2rQmviYnvsOq70wgywZd26_Iad_VrUUy6_qYMETydYnFqRot5uPiz89fbjRni7H7NhKbZTwUMnJ3t-_vbmFC2ISICSnG5LpNDVliQpda7zZGqUGyqJJp0AbTkRMcviFHwazw2ofv8R05wGZtgz9HZ_5xjLP3N_Nfg05E_qFPxqFtffcye1abLuKr-76bfTk6_Dyb58eLj59m-8d5xVWRcs6EKJFxWdcCeV2eWbCVQMGMrcVZSbnkaGllwNqpGqossKaW21LQEigFvpu92epeBv-jx5j0he-DGyw1K6liUopyOqDoFlUFH2PAWl-GdmXCWlPQm-T0Njk9JKc3yembgcO2nDhg3TmGB-XHSX8BVuCfsg</addsrcrecordid><sourcetype>Aggregation Database</sourcetype><iscdi>true</iscdi><recordtype>article</recordtype><pqid>2918277495</pqid></control><display><type>article</type><title>Catalytic Activity of Molecular Rhenium Sulfide Clusters [Re6S8(OH)6−n(H2O)n](4−n)− (n = 0, 2, 4, 6) with Retention of the Octahedral Metal Frameworks: Dehydrogenation and Dehydration of 1,4-Butanediol</title><source>Springer Nature - Complete Springer Journals</source><source>ProQuest Central</source><creator>Nagashima, Sayoko ; Furukawa, Shota ; Kamiguchi, Satoshi ; Kajio, Ryu ; Nagashima, Hiroshi ; Yamaguchi, Aritomo ; Shirai, Masayuki ; Kurokawa, Hideki ; Chihara, Teiji</creator><creatorcontrib>Nagashima, Sayoko ; Furukawa, Shota ; Kamiguchi, Satoshi ; Kajio, Ryu ; Nagashima, Hiroshi ; Yamaguchi, Aritomo ; Shirai, Masayuki ; Kurokawa, Hideki ; Chihara, Teiji</creatorcontrib><description>A series of molecular rhenium sulfide clusters [Re
6
S
8
(OH)
6−
n
(H
2
O)
n
]
(4−
n
)−
(
n
= 0, 2, 4, 6) catalyze dehydrogenation of alcohols, and hydrogenation of ketones and olefins in a hydrogen stream at 350 °C. The catalytic activities of the dianionic and neutral clusters (
n
= 2, 4) are lower than those of tetraanionic and dicationic clusters (
n
= 0, 6) for all the reactions. When 1,4-butanediol is allowed to react over K
4
[Re
6
S
8
(OH)
6
], dehydrogenation proceeds to yield 2-hydroxytetrahydrofuran and successively γ-butyrolactone above 300 °C. Over [Re
6
S
8
(H
2
O)
6
]SO
4
dehydration proceeds to yield tetrahydrofuran above 250 °C. The thermal activation mechanisms of these clusters were studied by powder X-ray diffraction analyses, Raman spectrometry, extended X-ray absorption fine structure spectrometry, thermogravimetry, and differential thermal analyses. The catalytically active site of K
4
[Re
6
S
8
(OH)
6
] is an uncoordinated metal site (Lewis acid site) developed by the loss of a water molecule from two hydroxo ligands. The active site of [Re
6
S
8
(H
2
O)
6
]SO
4
is a Brønsted acid site; the anhydrous aqua cluster dication disproportionates to a hydroxo cluster monocation and a proton. Both of the octahedral cluster frameworks are retained up to 500 °C.</description><identifier>ISSN: 1040-7278</identifier><identifier>EISSN: 1572-8862</identifier><identifier>DOI: 10.1007/s10876-014-0700-x</identifier><language>eng</language><publisher>Boston: Springer US</publisher><subject>Alcohols ; Alkenes ; Aqueous solutions ; Butanediol ; Catalysis ; Catalytic activity ; Chemistry ; Chemistry and Materials Science ; Clusters ; Dehydration ; Dehydrogenation ; Differential thermal analysis ; Fine structure ; Hydrogenation ; Inorganic Chemistry ; Ketones ; Lewis acid ; Ligands ; Nanochemistry ; Original Paper ; Oxidation ; Physical Chemistry ; Rhenium ; Spectrometry ; Temperature ; Tetrahydrofuran ; Thermogravimetry ; X ray absorption ; X ray powder diffraction</subject><ispartof>Journal of cluster science, 2014-09, Vol.25 (5), p.1203-1224</ispartof><rights>Springer Science+Business Media New York 2014</rights><rights>Springer Science+Business Media New York 2014.</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c386t-32449e237ff4e3f9bd0dc4e42adf4b91373ed1ca0dd58a0d76ef1d3d941901103</citedby><cites>FETCH-LOGICAL-c386t-32449e237ff4e3f9bd0dc4e42adf4b91373ed1ca0dd58a0d76ef1d3d941901103</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://link.springer.com/content/pdf/10.1007/s10876-014-0700-x$$EPDF$$P50$$Gspringer$$H</linktopdf><linktohtml>$$Uhttps://www.proquest.com/docview/2918277495?pq-origsite=primo$$EHTML$$P50$$Gproquest$$H</linktohtml><link.rule.ids>314,776,780,21367,27901,27902,33721,41464,42533,43781,51294</link.rule.ids></links><search><creatorcontrib>Nagashima, Sayoko</creatorcontrib><creatorcontrib>Furukawa, Shota</creatorcontrib><creatorcontrib>Kamiguchi, Satoshi</creatorcontrib><creatorcontrib>Kajio, Ryu</creatorcontrib><creatorcontrib>Nagashima, Hiroshi</creatorcontrib><creatorcontrib>Yamaguchi, Aritomo</creatorcontrib><creatorcontrib>Shirai, Masayuki</creatorcontrib><creatorcontrib>Kurokawa, Hideki</creatorcontrib><creatorcontrib>Chihara, Teiji</creatorcontrib><title>Catalytic Activity of Molecular Rhenium Sulfide Clusters [Re6S8(OH)6−n(H2O)n](4−n)− (n = 0, 2, 4, 6) with Retention of the Octahedral Metal Frameworks: Dehydrogenation and Dehydration of 1,4-Butanediol</title><title>Journal of cluster science</title><addtitle>J Clust Sci</addtitle><description>A series of molecular rhenium sulfide clusters [Re
6
S
8
(OH)
6−
n
(H
2
O)
n
]
(4−
n
)−
(
n
= 0, 2, 4, 6) catalyze dehydrogenation of alcohols, and hydrogenation of ketones and olefins in a hydrogen stream at 350 °C. The catalytic activities of the dianionic and neutral clusters (
n
= 2, 4) are lower than those of tetraanionic and dicationic clusters (
n
= 0, 6) for all the reactions. When 1,4-butanediol is allowed to react over K
4
[Re
6
S
8
(OH)
6
], dehydrogenation proceeds to yield 2-hydroxytetrahydrofuran and successively γ-butyrolactone above 300 °C. Over [Re
6
S
8
(H
2
O)
6
]SO
4
dehydration proceeds to yield tetrahydrofuran above 250 °C. The thermal activation mechanisms of these clusters were studied by powder X-ray diffraction analyses, Raman spectrometry, extended X-ray absorption fine structure spectrometry, thermogravimetry, and differential thermal analyses. The catalytically active site of K
4
[Re
6
S
8
(OH)
6
] is an uncoordinated metal site (Lewis acid site) developed by the loss of a water molecule from two hydroxo ligands. The active site of [Re
6
S
8
(H
2
O)
6
]SO
4
is a Brønsted acid site; the anhydrous aqua cluster dication disproportionates to a hydroxo cluster monocation and a proton. Both of the octahedral cluster frameworks are retained up to 500 °C.</description><subject>Alcohols</subject><subject>Alkenes</subject><subject>Aqueous solutions</subject><subject>Butanediol</subject><subject>Catalysis</subject><subject>Catalytic activity</subject><subject>Chemistry</subject><subject>Chemistry and Materials Science</subject><subject>Clusters</subject><subject>Dehydration</subject><subject>Dehydrogenation</subject><subject>Differential thermal analysis</subject><subject>Fine structure</subject><subject>Hydrogenation</subject><subject>Inorganic Chemistry</subject><subject>Ketones</subject><subject>Lewis acid</subject><subject>Ligands</subject><subject>Nanochemistry</subject><subject>Original Paper</subject><subject>Oxidation</subject><subject>Physical Chemistry</subject><subject>Rhenium</subject><subject>Spectrometry</subject><subject>Temperature</subject><subject>Tetrahydrofuran</subject><subject>Thermogravimetry</subject><subject>X ray absorption</subject><subject>X ray powder diffraction</subject><issn>1040-7278</issn><issn>1572-8862</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2014</creationdate><recordtype>article</recordtype><sourceid>BENPR</sourceid><recordid>eNp1UU1uEzEUHiGQKIUDsLPEJpEy5fknYw8Si5K2BKlVpBRWCFnu-E1nysQutqdtbsCaE_QsvQFX4CRMSFFX3bw_fT9P-rLsNYU9CiDfRgpKFjlQkYMEyG-eZDt0KlmuVMGeDjMIyCWT6nn2IsYLACgV5zvZ75lJpluntiL7VWqv2rQmviYnvsOq70wgywZd26_Iad_VrUUy6_qYMETydYnFqRot5uPiz89fbjRni7H7NhKbZTwUMnJ3t-_vbmFC2ISICSnG5LpNDVliQpda7zZGqUGyqJJp0AbTkRMcviFHwazw2ofv8R05wGZtgz9HZ_5xjLP3N_Nfg05E_qFPxqFtffcye1abLuKr-76bfTk6_Dyb58eLj59m-8d5xVWRcs6EKJFxWdcCeV2eWbCVQMGMrcVZSbnkaGllwNqpGqossKaW21LQEigFvpu92epeBv-jx5j0he-DGyw1K6liUopyOqDoFlUFH2PAWl-GdmXCWlPQm-T0Njk9JKc3yembgcO2nDhg3TmGB-XHSX8BVuCfsg</recordid><startdate>20140901</startdate><enddate>20140901</enddate><creator>Nagashima, Sayoko</creator><creator>Furukawa, Shota</creator><creator>Kamiguchi, Satoshi</creator><creator>Kajio, Ryu</creator><creator>Nagashima, Hiroshi</creator><creator>Yamaguchi, Aritomo</creator><creator>Shirai, Masayuki</creator><creator>Kurokawa, Hideki</creator><creator>Chihara, Teiji</creator><general>Springer US</general><general>Springer Nature B.V</general><scope>AAYXX</scope><scope>CITATION</scope><scope>3V.</scope><scope>7XB</scope><scope>88I</scope><scope>8FE</scope><scope>8FG</scope><scope>8FK</scope><scope>ABJCF</scope><scope>ABUWG</scope><scope>AFKRA</scope><scope>ARAPS</scope><scope>AZQEC</scope><scope>BENPR</scope><scope>BGLVJ</scope><scope>CCPQU</scope><scope>D1I</scope><scope>DWQXO</scope><scope>GNUQQ</scope><scope>HCIFZ</scope><scope>KB.</scope><scope>M2P</scope><scope>P5Z</scope><scope>P62</scope><scope>PDBOC</scope><scope>PQEST</scope><scope>PQQKQ</scope><scope>PQUKI</scope><scope>Q9U</scope></search><sort><creationdate>20140901</creationdate><title>Catalytic Activity of Molecular Rhenium Sulfide Clusters [Re6S8(OH)6−n(H2O)n](4−n)− (n = 0, 2, 4, 6) with Retention of the Octahedral Metal Frameworks: Dehydrogenation and Dehydration of 1,4-Butanediol</title><author>Nagashima, Sayoko ; Furukawa, Shota ; Kamiguchi, Satoshi ; Kajio, Ryu ; Nagashima, Hiroshi ; Yamaguchi, Aritomo ; Shirai, Masayuki ; Kurokawa, Hideki ; Chihara, Teiji</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c386t-32449e237ff4e3f9bd0dc4e42adf4b91373ed1ca0dd58a0d76ef1d3d941901103</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2014</creationdate><topic>Alcohols</topic><topic>Alkenes</topic><topic>Aqueous solutions</topic><topic>Butanediol</topic><topic>Catalysis</topic><topic>Catalytic activity</topic><topic>Chemistry</topic><topic>Chemistry and Materials Science</topic><topic>Clusters</topic><topic>Dehydration</topic><topic>Dehydrogenation</topic><topic>Differential thermal analysis</topic><topic>Fine structure</topic><topic>Hydrogenation</topic><topic>Inorganic Chemistry</topic><topic>Ketones</topic><topic>Lewis acid</topic><topic>Ligands</topic><topic>Nanochemistry</topic><topic>Original Paper</topic><topic>Oxidation</topic><topic>Physical Chemistry</topic><topic>Rhenium</topic><topic>Spectrometry</topic><topic>Temperature</topic><topic>Tetrahydrofuran</topic><topic>Thermogravimetry</topic><topic>X ray absorption</topic><topic>X ray powder diffraction</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Nagashima, Sayoko</creatorcontrib><creatorcontrib>Furukawa, Shota</creatorcontrib><creatorcontrib>Kamiguchi, Satoshi</creatorcontrib><creatorcontrib>Kajio, Ryu</creatorcontrib><creatorcontrib>Nagashima, Hiroshi</creatorcontrib><creatorcontrib>Yamaguchi, Aritomo</creatorcontrib><creatorcontrib>Shirai, Masayuki</creatorcontrib><creatorcontrib>Kurokawa, Hideki</creatorcontrib><creatorcontrib>Chihara, Teiji</creatorcontrib><collection>CrossRef</collection><collection>ProQuest Central (Corporate)</collection><collection>ProQuest Central (purchase pre-March 2016)</collection><collection>Science Database (Alumni Edition)</collection><collection>ProQuest SciTech Collection</collection><collection>ProQuest Technology Collection</collection><collection>ProQuest Central (Alumni) (purchase pre-March 2016)</collection><collection>Materials Science & Engineering Collection</collection><collection>ProQuest Central (Alumni Edition)</collection><collection>ProQuest Central UK/Ireland</collection><collection>Advanced Technologies & Aerospace Collection</collection><collection>ProQuest Central Essentials</collection><collection>ProQuest Central</collection><collection>Technology Collection</collection><collection>ProQuest One Community College</collection><collection>ProQuest Materials Science Collection</collection><collection>ProQuest Central Korea</collection><collection>ProQuest Central Student</collection><collection>SciTech Premium Collection</collection><collection>Materials Science Database</collection><collection>Science Database</collection><collection>Advanced Technologies & Aerospace Database</collection><collection>ProQuest Advanced Technologies & Aerospace Collection</collection><collection>Materials Science Collection</collection><collection>ProQuest One Academic Eastern Edition (DO NOT USE)</collection><collection>ProQuest One Academic</collection><collection>ProQuest One Academic UKI Edition</collection><collection>ProQuest Central Basic</collection><jtitle>Journal of cluster science</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Nagashima, Sayoko</au><au>Furukawa, Shota</au><au>Kamiguchi, Satoshi</au><au>Kajio, Ryu</au><au>Nagashima, Hiroshi</au><au>Yamaguchi, Aritomo</au><au>Shirai, Masayuki</au><au>Kurokawa, Hideki</au><au>Chihara, Teiji</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Catalytic Activity of Molecular Rhenium Sulfide Clusters [Re6S8(OH)6−n(H2O)n](4−n)− (n = 0, 2, 4, 6) with Retention of the Octahedral Metal Frameworks: Dehydrogenation and Dehydration of 1,4-Butanediol</atitle><jtitle>Journal of cluster science</jtitle><stitle>J Clust Sci</stitle><date>2014-09-01</date><risdate>2014</risdate><volume>25</volume><issue>5</issue><spage>1203</spage><epage>1224</epage><pages>1203-1224</pages><issn>1040-7278</issn><eissn>1572-8862</eissn><abstract>A series of molecular rhenium sulfide clusters [Re
6
S
8
(OH)
6−
n
(H
2
O)
n
]
(4−
n
)−
(
n
= 0, 2, 4, 6) catalyze dehydrogenation of alcohols, and hydrogenation of ketones and olefins in a hydrogen stream at 350 °C. The catalytic activities of the dianionic and neutral clusters (
n
= 2, 4) are lower than those of tetraanionic and dicationic clusters (
n
= 0, 6) for all the reactions. When 1,4-butanediol is allowed to react over K
4
[Re
6
S
8
(OH)
6
], dehydrogenation proceeds to yield 2-hydroxytetrahydrofuran and successively γ-butyrolactone above 300 °C. Over [Re
6
S
8
(H
2
O)
6
]SO
4
dehydration proceeds to yield tetrahydrofuran above 250 °C. The thermal activation mechanisms of these clusters were studied by powder X-ray diffraction analyses, Raman spectrometry, extended X-ray absorption fine structure spectrometry, thermogravimetry, and differential thermal analyses. The catalytically active site of K
4
[Re
6
S
8
(OH)
6
] is an uncoordinated metal site (Lewis acid site) developed by the loss of a water molecule from two hydroxo ligands. The active site of [Re
6
S
8
(H
2
O)
6
]SO
4
is a Brønsted acid site; the anhydrous aqua cluster dication disproportionates to a hydroxo cluster monocation and a proton. Both of the octahedral cluster frameworks are retained up to 500 °C.</abstract><cop>Boston</cop><pub>Springer US</pub><doi>10.1007/s10876-014-0700-x</doi><tpages>22</tpages></addata></record> |
| fulltext | fulltext |
| identifier | ISSN: 1040-7278 |
| ispartof | Journal of cluster science, 2014-09, Vol.25 (5), p.1203-1224 |
| issn | 1040-7278 1572-8862 |
| language | eng |
| recordid | cdi_proquest_journals_2918277495 |
| source | Springer Nature - Complete Springer Journals; ProQuest Central |
| subjects | Alcohols Alkenes Aqueous solutions Butanediol Catalysis Catalytic activity Chemistry Chemistry and Materials Science Clusters Dehydration Dehydrogenation Differential thermal analysis Fine structure Hydrogenation Inorganic Chemistry Ketones Lewis acid Ligands Nanochemistry Original Paper Oxidation Physical Chemistry Rhenium Spectrometry Temperature Tetrahydrofuran Thermogravimetry X ray absorption X ray powder diffraction |
| title | Catalytic Activity of Molecular Rhenium Sulfide Clusters [Re6S8(OH)6−n(H2O)n](4−n)− (n = 0, 2, 4, 6) with Retention of the Octahedral Metal Frameworks: Dehydrogenation and Dehydration of 1,4-Butanediol |
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