Ceria-supported ruthenium nanoparticles as highly active and long-lived catalysts in hydrogen generation from the hydrolysis of ammonia borane
Ruthenium(0) nanoparticles supported on ceria (Ru 0 /CeO 2 ) were in situ generated from the reduction of ruthenium( iii ) ions impregnated on ceria during the hydrolysis of ammonia borane. Ru 0 /CeO 2 was isolated from the reaction solution by centrifugation and characterized by ICP-OES, BET, XRD,...
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Veröffentlicht in: | Dalton transactions : an international journal of inorganic chemistry 2016-07, Vol.45 (27), p.1969-1978 |
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container_end_page | 1978 |
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container_issue | 27 |
container_start_page | 1969 |
container_title | Dalton transactions : an international journal of inorganic chemistry |
container_volume | 45 |
creator | Akbayrak, Serdar Tonbul, Yalç n Özkar, Saim |
description | Ruthenium(0) nanoparticles supported on ceria (Ru
0
/CeO
2
) were
in situ
generated from the reduction of ruthenium(
iii
) ions impregnated on ceria during the hydrolysis of ammonia borane. Ru
0
/CeO
2
was isolated from the reaction solution by centrifugation and characterized by ICP-OES, BET, XRD, TEM, SEM-EDS and XPS techniques. All the results reveal that ruthenium(0) nanoparticles were successfully supported on ceria and the resulting Ru
0
/CeO
2
is a highly active, reusable and long-lived catalyst for hydrogen generation from the hydrolysis of ammonia borane with a turnover frequency value of 361 min
−1
. The reusability tests reveal that Ru
0
/CeO
2
is still active in the subsequent runs of hydrolysis of ammonia borane preserving 60% of the initial catalytic activity even after the fifth run. Ru
0
/CeO
2
provides a superior catalytic lifetime (TTO = 135 100) in hydrogen generation from the hydrolysis of ammonia borane at 25.0 ± 0.1 °C before deactivation. The work reported here includes the formation kinetics of ruthenium(0) nanoparticles. The rate constants for the slow nucleation and autocatalytic surface growth of ruthenium(0) nanoparticles were obtained using hydrogen evolution as a reporter reaction. An evaluation of rate constants at various temperatures enabled the estimation of activation energies for both the reactions,
E
a
= 60 ± 7 kJ mol
−1
for the nucleation and
E
a
= 47 ± 2 kJ mol
−1
for the autocatalytic surface growth of ruthenium(0) nanoparticles, as well as the activation energy of
E
a
= 51 ± 2 kJ mol
−1
for the catalytic hydrolysis of ammonia borane.
Ruthenium(0) nanoparticles supported on ceria (Ru
0
/CeO
2
) were
in situ
generated from the reduction of ruthenium(
iii
) ions impregnated on ceria during the hydrolysis of ammonia borane. |
doi_str_mv | 10.1039/c6dt01117a |
format | Article |
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0
/CeO
2
) were
in situ
generated from the reduction of ruthenium(
iii
) ions impregnated on ceria during the hydrolysis of ammonia borane. Ru
0
/CeO
2
was isolated from the reaction solution by centrifugation and characterized by ICP-OES, BET, XRD, TEM, SEM-EDS and XPS techniques. All the results reveal that ruthenium(0) nanoparticles were successfully supported on ceria and the resulting Ru
0
/CeO
2
is a highly active, reusable and long-lived catalyst for hydrogen generation from the hydrolysis of ammonia borane with a turnover frequency value of 361 min
−1
. The reusability tests reveal that Ru
0
/CeO
2
is still active in the subsequent runs of hydrolysis of ammonia borane preserving 60% of the initial catalytic activity even after the fifth run. Ru
0
/CeO
2
provides a superior catalytic lifetime (TTO = 135 100) in hydrogen generation from the hydrolysis of ammonia borane at 25.0 ± 0.1 °C before deactivation. The work reported here includes the formation kinetics of ruthenium(0) nanoparticles. The rate constants for the slow nucleation and autocatalytic surface growth of ruthenium(0) nanoparticles were obtained using hydrogen evolution as a reporter reaction. An evaluation of rate constants at various temperatures enabled the estimation of activation energies for both the reactions,
E
a
= 60 ± 7 kJ mol
−1
for the nucleation and
E
a
= 47 ± 2 kJ mol
−1
for the autocatalytic surface growth of ruthenium(0) nanoparticles, as well as the activation energy of
E
a
= 51 ± 2 kJ mol
−1
for the catalytic hydrolysis of ammonia borane.
Ruthenium(0) nanoparticles supported on ceria (Ru
0
/CeO
2
) were
in situ
generated from the reduction of ruthenium(
iii
) ions impregnated on ceria during the hydrolysis of ammonia borane.</description><identifier>ISSN: 1477-9226</identifier><identifier>EISSN: 1477-9234</identifier><identifier>DOI: 10.1039/c6dt01117a</identifier><identifier>PMID: 27302302</identifier><language>eng</language><publisher>England</publisher><subject>Ammonia ; Boranes ; Catalysis ; Catalysts ; Cerium oxide ; Hydrogen ; Hydrolysis ; Nanoparticles</subject><ispartof>Dalton transactions : an international journal of inorganic chemistry, 2016-07, Vol.45 (27), p.1969-1978</ispartof><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c342t-1edfeb3f7d16fb2cb86b80c8e47325816dbb838abb1de84e035360f64348e8bc3</citedby><cites>FETCH-LOGICAL-c342t-1edfeb3f7d16fb2cb86b80c8e47325816dbb838abb1de84e035360f64348e8bc3</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,777,781,27905,27906</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/27302302$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Akbayrak, Serdar</creatorcontrib><creatorcontrib>Tonbul, Yalç n</creatorcontrib><creatorcontrib>Özkar, Saim</creatorcontrib><title>Ceria-supported ruthenium nanoparticles as highly active and long-lived catalysts in hydrogen generation from the hydrolysis of ammonia borane</title><title>Dalton transactions : an international journal of inorganic chemistry</title><addtitle>Dalton Trans</addtitle><description>Ruthenium(0) nanoparticles supported on ceria (Ru
0
/CeO
2
) were
in situ
generated from the reduction of ruthenium(
iii
) ions impregnated on ceria during the hydrolysis of ammonia borane. Ru
0
/CeO
2
was isolated from the reaction solution by centrifugation and characterized by ICP-OES, BET, XRD, TEM, SEM-EDS and XPS techniques. All the results reveal that ruthenium(0) nanoparticles were successfully supported on ceria and the resulting Ru
0
/CeO
2
is a highly active, reusable and long-lived catalyst for hydrogen generation from the hydrolysis of ammonia borane with a turnover frequency value of 361 min
−1
. The reusability tests reveal that Ru
0
/CeO
2
is still active in the subsequent runs of hydrolysis of ammonia borane preserving 60% of the initial catalytic activity even after the fifth run. Ru
0
/CeO
2
provides a superior catalytic lifetime (TTO = 135 100) in hydrogen generation from the hydrolysis of ammonia borane at 25.0 ± 0.1 °C before deactivation. The work reported here includes the formation kinetics of ruthenium(0) nanoparticles. The rate constants for the slow nucleation and autocatalytic surface growth of ruthenium(0) nanoparticles were obtained using hydrogen evolution as a reporter reaction. An evaluation of rate constants at various temperatures enabled the estimation of activation energies for both the reactions,
E
a
= 60 ± 7 kJ mol
−1
for the nucleation and
E
a
= 47 ± 2 kJ mol
−1
for the autocatalytic surface growth of ruthenium(0) nanoparticles, as well as the activation energy of
E
a
= 51 ± 2 kJ mol
−1
for the catalytic hydrolysis of ammonia borane.
Ruthenium(0) nanoparticles supported on ceria (Ru
0
/CeO
2
) were
in situ
generated from the reduction of ruthenium(
iii
) ions impregnated on ceria during the hydrolysis of ammonia borane.</description><subject>Ammonia</subject><subject>Boranes</subject><subject>Catalysis</subject><subject>Catalysts</subject><subject>Cerium oxide</subject><subject>Hydrogen</subject><subject>Hydrolysis</subject><subject>Nanoparticles</subject><issn>1477-9226</issn><issn>1477-9234</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2016</creationdate><recordtype>article</recordtype><recordid>eNqNkU1r3DAQhkVIaJJtL7kn6FgKTvThlbXHxW3TQCCX9Gz0Md5VsCVHkgv7J_qbo2ST7bUww8wwD-8MvAhdUHJNCV_dGGEzoZQ26gid0bppqhXj9fGhZ-IUnaf0RAhjZMk-oVPWcMJKnKG_LUSnqjRPU4gZLI5z3oJ384i98mFSMTszQMIq4a3bbIcdVia7P4CVt3gIflMNZbLYqKyGXcoJO4-3OxvDBjwuCVFlFzzuYxhx0d4vC-oSDj1W4xi8U1iHqDx8Rie9GhJ8ea8L9Pvnj8f2V3X_cHvXru8rw2uWKwq2B837xlLRa2a0FFoSI6FuOFtKKqzWkkulNbUgayB8yQXpRc1rCVIbvkBf97pTDM8zpNyNLhkYhvJDmFNHpaiXQqyI_A-UsHJWilVBv-1RE0NKEfpuim5UcddR0r1a1bXi--ObVesCX73rznoEe0A_vCnA5R6IyRy2_7zmLx8Zm_E</recordid><startdate>20160705</startdate><enddate>20160705</enddate><creator>Akbayrak, Serdar</creator><creator>Tonbul, Yalç n</creator><creator>Özkar, Saim</creator><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7X8</scope><scope>7SR</scope><scope>7U5</scope><scope>8BQ</scope><scope>8FD</scope><scope>JG9</scope><scope>L7M</scope></search><sort><creationdate>20160705</creationdate><title>Ceria-supported ruthenium nanoparticles as highly active and long-lived catalysts in hydrogen generation from the hydrolysis of ammonia borane</title><author>Akbayrak, Serdar ; Tonbul, Yalç n ; Özkar, Saim</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c342t-1edfeb3f7d16fb2cb86b80c8e47325816dbb838abb1de84e035360f64348e8bc3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2016</creationdate><topic>Ammonia</topic><topic>Boranes</topic><topic>Catalysis</topic><topic>Catalysts</topic><topic>Cerium oxide</topic><topic>Hydrogen</topic><topic>Hydrolysis</topic><topic>Nanoparticles</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Akbayrak, Serdar</creatorcontrib><creatorcontrib>Tonbul, Yalç n</creatorcontrib><creatorcontrib>Özkar, Saim</creatorcontrib><collection>PubMed</collection><collection>CrossRef</collection><collection>MEDLINE - Academic</collection><collection>Engineered Materials Abstracts</collection><collection>Solid State and Superconductivity Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Materials Research Database</collection><collection>Advanced Technologies Database with Aerospace</collection><jtitle>Dalton transactions : an international journal of inorganic chemistry</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Akbayrak, Serdar</au><au>Tonbul, Yalç n</au><au>Özkar, Saim</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Ceria-supported ruthenium nanoparticles as highly active and long-lived catalysts in hydrogen generation from the hydrolysis of ammonia borane</atitle><jtitle>Dalton transactions : an international journal of inorganic chemistry</jtitle><addtitle>Dalton Trans</addtitle><date>2016-07-05</date><risdate>2016</risdate><volume>45</volume><issue>27</issue><spage>1969</spage><epage>1978</epage><pages>1969-1978</pages><issn>1477-9226</issn><eissn>1477-9234</eissn><abstract>Ruthenium(0) nanoparticles supported on ceria (Ru
0
/CeO
2
) were
in situ
generated from the reduction of ruthenium(
iii
) ions impregnated on ceria during the hydrolysis of ammonia borane. Ru
0
/CeO
2
was isolated from the reaction solution by centrifugation and characterized by ICP-OES, BET, XRD, TEM, SEM-EDS and XPS techniques. All the results reveal that ruthenium(0) nanoparticles were successfully supported on ceria and the resulting Ru
0
/CeO
2
is a highly active, reusable and long-lived catalyst for hydrogen generation from the hydrolysis of ammonia borane with a turnover frequency value of 361 min
−1
. The reusability tests reveal that Ru
0
/CeO
2
is still active in the subsequent runs of hydrolysis of ammonia borane preserving 60% of the initial catalytic activity even after the fifth run. Ru
0
/CeO
2
provides a superior catalytic lifetime (TTO = 135 100) in hydrogen generation from the hydrolysis of ammonia borane at 25.0 ± 0.1 °C before deactivation. The work reported here includes the formation kinetics of ruthenium(0) nanoparticles. The rate constants for the slow nucleation and autocatalytic surface growth of ruthenium(0) nanoparticles were obtained using hydrogen evolution as a reporter reaction. An evaluation of rate constants at various temperatures enabled the estimation of activation energies for both the reactions,
E
a
= 60 ± 7 kJ mol
−1
for the nucleation and
E
a
= 47 ± 2 kJ mol
−1
for the autocatalytic surface growth of ruthenium(0) nanoparticles, as well as the activation energy of
E
a
= 51 ± 2 kJ mol
−1
for the catalytic hydrolysis of ammonia borane.
Ruthenium(0) nanoparticles supported on ceria (Ru
0
/CeO
2
) were
in situ
generated from the reduction of ruthenium(
iii
) ions impregnated on ceria during the hydrolysis of ammonia borane.</abstract><cop>England</cop><pmid>27302302</pmid><doi>10.1039/c6dt01117a</doi><tpages>1</tpages></addata></record> |
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issn | 1477-9226 1477-9234 |
language | eng |
recordid | cdi_proquest_miscellaneous_1802473869 |
source | Royal Society Of Chemistry Journals 2008-; Alma/SFX Local Collection |
subjects | Ammonia Boranes Catalysis Catalysts Cerium oxide Hydrogen Hydrolysis Nanoparticles |
title | Ceria-supported ruthenium nanoparticles as highly active and long-lived catalysts in hydrogen generation from the hydrolysis of ammonia borane |
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