f‐ block MOFs: A Pathway to Heterometallic Transuranics
Abstract A novel series of heterometallic f ‐block‐frameworks including the first examples of transuranic heterometallic 238 U/ 239 Pu‐metal–organic frameworks (MOFs) and a novel monometallic 239 Pu‐analog are reported. In combination with theoretical calculations, we probed the kinetics and thermod...
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| Veröffentlicht in: | Angewandte Chemie (International ed.) 2022-12, Vol.62 (5) |
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| creator | Park, Kyoung Chul Kittikhunnatham, Preecha Lim, Jaewoong Thaggard, Grace C. Liu, Yuan Martin, Corey R. Leith, Gabrielle A. Toler, Donald J. Ta, An T. Birkner, Nancy Lehman‐Andino, Ingrid Hernandez‐Jimenez, Alejandra Morrison, Gregory Amoroso, Jake W. zur Loye, Hans‐Conrad DiPrete, Dave P. Smith, Mark D. Brinkman, Kyle S. Phillpot, Simon R. Shustova, Natalia B. |
| description | Abstract
A novel series of heterometallic
f
‐block‐frameworks including the first examples of transuranic heterometallic
238
U/
239
Pu‐metal–organic frameworks (MOFs) and a novel monometallic
239
Pu‐analog are reported. In combination with theoretical calculations, we probed the kinetics and thermodynamics of heterometallic actinide(An)‐MOF formation and reported the first value of a U‐to‐Th transmetallation rate. We concluded that formation of uranyl species could be a driving force for solid‐state metathesis. Density of states near the Fermi edge, enthalpy of formation, band gap, proton affinity, and thermal/chemical stability were probed as a function of metal ratios. Furthermore, we achieved 97 % of the theoretical maximum capacity for An‐integration. These studies shed light on fundamental aspects of actinide chemistry and also foreshadow avenues for the development of emerging classes of An‐containing materials, including radioisotope thermoelectric generators or metalloradiopharmaceuticals. |
| format | Article |
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A novel series of heterometallic
f
‐block‐frameworks including the first examples of transuranic heterometallic
238
U/
239
Pu‐metal–organic frameworks (MOFs) and a novel monometallic
239
Pu‐analog are reported. In combination with theoretical calculations, we probed the kinetics and thermodynamics of heterometallic actinide(An)‐MOF formation and reported the first value of a U‐to‐Th transmetallation rate. We concluded that formation of uranyl species could be a driving force for solid‐state metathesis. Density of states near the Fermi edge, enthalpy of formation, band gap, proton affinity, and thermal/chemical stability were probed as a function of metal ratios. Furthermore, we achieved 97 % of the theoretical maximum capacity for An‐integration. These studies shed light on fundamental aspects of actinide chemistry and also foreshadow avenues for the development of emerging classes of An‐containing materials, including radioisotope thermoelectric generators or metalloradiopharmaceuticals.</description><identifier>ISSN: 1433-7851</identifier><identifier>EISSN: 1521-3773</identifier><language>eng</language><publisher>Germany: Wiley Blackwell (John Wiley & Sons)</publisher><ispartof>Angewandte Chemie (International ed.), 2022-12, Vol.62 (5)</ispartof><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><orcidid>0000000222191253 ; 0000000245570870 ; 0000000180241661 ; 0000000339734207 ; 0000000227678343 ; 0000000339521949 ; 000000033804487X ; 0000000277746535</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>230,314,776,780,881</link.rule.ids><backlink>$$Uhttps://www.osti.gov/biblio/1910285$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Park, Kyoung Chul</creatorcontrib><creatorcontrib>Kittikhunnatham, Preecha</creatorcontrib><creatorcontrib>Lim, Jaewoong</creatorcontrib><creatorcontrib>Thaggard, Grace C.</creatorcontrib><creatorcontrib>Liu, Yuan</creatorcontrib><creatorcontrib>Martin, Corey R.</creatorcontrib><creatorcontrib>Leith, Gabrielle A.</creatorcontrib><creatorcontrib>Toler, Donald J.</creatorcontrib><creatorcontrib>Ta, An T.</creatorcontrib><creatorcontrib>Birkner, Nancy</creatorcontrib><creatorcontrib>Lehman‐Andino, Ingrid</creatorcontrib><creatorcontrib>Hernandez‐Jimenez, Alejandra</creatorcontrib><creatorcontrib>Morrison, Gregory</creatorcontrib><creatorcontrib>Amoroso, Jake W.</creatorcontrib><creatorcontrib>zur Loye, Hans‐Conrad</creatorcontrib><creatorcontrib>DiPrete, Dave P.</creatorcontrib><creatorcontrib>Smith, Mark D.</creatorcontrib><creatorcontrib>Brinkman, Kyle S.</creatorcontrib><creatorcontrib>Phillpot, Simon R.</creatorcontrib><creatorcontrib>Shustova, Natalia B.</creatorcontrib><title>f‐ block MOFs: A Pathway to Heterometallic Transuranics</title><title>Angewandte Chemie (International ed.)</title><description>Abstract
A novel series of heterometallic
f
‐block‐frameworks including the first examples of transuranic heterometallic
238
U/
239
Pu‐metal–organic frameworks (MOFs) and a novel monometallic
239
Pu‐analog are reported. In combination with theoretical calculations, we probed the kinetics and thermodynamics of heterometallic actinide(An)‐MOF formation and reported the first value of a U‐to‐Th transmetallation rate. We concluded that formation of uranyl species could be a driving force for solid‐state metathesis. Density of states near the Fermi edge, enthalpy of formation, band gap, proton affinity, and thermal/chemical stability were probed as a function of metal ratios. Furthermore, we achieved 97 % of the theoretical maximum capacity for An‐integration. These studies shed light on fundamental aspects of actinide chemistry and also foreshadow avenues for the development of emerging classes of An‐containing materials, including radioisotope thermoelectric generators or metalloradiopharmaceuticals.</description><issn>1433-7851</issn><issn>1521-3773</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2022</creationdate><recordtype>article</recordtype><recordid>eNpjYuA0NDUy1DU2NzdmAbJNjI11zS1MDTkYuIqLswwMjCwsDMw4GSzTHjVMUEjKyU_OVvD1dyu2UnBUCEgsyShPrFQoyVfwSC1JLcrPTS1JzMnJTFYIKUrMKy4FEpnJxTwMrGmJOcWpvFCam0HJzTXE2UM3v7gkM744ObMkNTkjOT8vLzW5JN7Q0hBoo6kxUYoAEMs3zg</recordid><startdate>20221219</startdate><enddate>20221219</enddate><creator>Park, Kyoung Chul</creator><creator>Kittikhunnatham, Preecha</creator><creator>Lim, Jaewoong</creator><creator>Thaggard, Grace C.</creator><creator>Liu, Yuan</creator><creator>Martin, Corey R.</creator><creator>Leith, Gabrielle A.</creator><creator>Toler, Donald J.</creator><creator>Ta, An T.</creator><creator>Birkner, Nancy</creator><creator>Lehman‐Andino, Ingrid</creator><creator>Hernandez‐Jimenez, Alejandra</creator><creator>Morrison, Gregory</creator><creator>Amoroso, Jake W.</creator><creator>zur Loye, Hans‐Conrad</creator><creator>DiPrete, Dave P.</creator><creator>Smith, Mark D.</creator><creator>Brinkman, Kyle S.</creator><creator>Phillpot, Simon R.</creator><creator>Shustova, Natalia B.</creator><general>Wiley Blackwell (John Wiley & Sons)</general><scope>OTOTI</scope><orcidid>https://orcid.org/0000000222191253</orcidid><orcidid>https://orcid.org/0000000245570870</orcidid><orcidid>https://orcid.org/0000000180241661</orcidid><orcidid>https://orcid.org/0000000339734207</orcidid><orcidid>https://orcid.org/0000000227678343</orcidid><orcidid>https://orcid.org/0000000339521949</orcidid><orcidid>https://orcid.org/000000033804487X</orcidid><orcidid>https://orcid.org/0000000277746535</orcidid></search><sort><creationdate>20221219</creationdate><title>f‐ block MOFs: A Pathway to Heterometallic Transuranics</title><author>Park, Kyoung Chul ; Kittikhunnatham, Preecha ; Lim, Jaewoong ; Thaggard, Grace C. ; Liu, Yuan ; Martin, Corey R. ; Leith, Gabrielle A. ; Toler, Donald J. ; Ta, An T. ; Birkner, Nancy ; Lehman‐Andino, Ingrid ; Hernandez‐Jimenez, Alejandra ; Morrison, Gregory ; Amoroso, Jake W. ; zur Loye, Hans‐Conrad ; DiPrete, Dave P. ; Smith, Mark D. ; Brinkman, Kyle S. ; Phillpot, Simon R. ; Shustova, Natalia B.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-osti_scitechconnect_19102853</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2022</creationdate><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Park, Kyoung Chul</creatorcontrib><creatorcontrib>Kittikhunnatham, Preecha</creatorcontrib><creatorcontrib>Lim, Jaewoong</creatorcontrib><creatorcontrib>Thaggard, Grace C.</creatorcontrib><creatorcontrib>Liu, Yuan</creatorcontrib><creatorcontrib>Martin, Corey R.</creatorcontrib><creatorcontrib>Leith, Gabrielle A.</creatorcontrib><creatorcontrib>Toler, Donald J.</creatorcontrib><creatorcontrib>Ta, An T.</creatorcontrib><creatorcontrib>Birkner, Nancy</creatorcontrib><creatorcontrib>Lehman‐Andino, Ingrid</creatorcontrib><creatorcontrib>Hernandez‐Jimenez, Alejandra</creatorcontrib><creatorcontrib>Morrison, Gregory</creatorcontrib><creatorcontrib>Amoroso, Jake W.</creatorcontrib><creatorcontrib>zur Loye, Hans‐Conrad</creatorcontrib><creatorcontrib>DiPrete, Dave P.</creatorcontrib><creatorcontrib>Smith, Mark D.</creatorcontrib><creatorcontrib>Brinkman, Kyle S.</creatorcontrib><creatorcontrib>Phillpot, Simon R.</creatorcontrib><creatorcontrib>Shustova, Natalia B.</creatorcontrib><collection>OSTI.GOV</collection><jtitle>Angewandte Chemie (International ed.)</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Park, Kyoung Chul</au><au>Kittikhunnatham, Preecha</au><au>Lim, Jaewoong</au><au>Thaggard, Grace C.</au><au>Liu, Yuan</au><au>Martin, Corey R.</au><au>Leith, Gabrielle A.</au><au>Toler, Donald J.</au><au>Ta, An T.</au><au>Birkner, Nancy</au><au>Lehman‐Andino, Ingrid</au><au>Hernandez‐Jimenez, Alejandra</au><au>Morrison, Gregory</au><au>Amoroso, Jake W.</au><au>zur Loye, Hans‐Conrad</au><au>DiPrete, Dave P.</au><au>Smith, Mark D.</au><au>Brinkman, Kyle S.</au><au>Phillpot, Simon R.</au><au>Shustova, Natalia B.</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>f‐ block MOFs: A Pathway to Heterometallic Transuranics</atitle><jtitle>Angewandte Chemie (International ed.)</jtitle><date>2022-12-19</date><risdate>2022</risdate><volume>62</volume><issue>5</issue><issn>1433-7851</issn><eissn>1521-3773</eissn><abstract>Abstract
A novel series of heterometallic
f
‐block‐frameworks including the first examples of transuranic heterometallic
238
U/
239
Pu‐metal–organic frameworks (MOFs) and a novel monometallic
239
Pu‐analog are reported. In combination with theoretical calculations, we probed the kinetics and thermodynamics of heterometallic actinide(An)‐MOF formation and reported the first value of a U‐to‐Th transmetallation rate. We concluded that formation of uranyl species could be a driving force for solid‐state metathesis. Density of states near the Fermi edge, enthalpy of formation, band gap, proton affinity, and thermal/chemical stability were probed as a function of metal ratios. Furthermore, we achieved 97 % of the theoretical maximum capacity for An‐integration. These studies shed light on fundamental aspects of actinide chemistry and also foreshadow avenues for the development of emerging classes of An‐containing materials, including radioisotope thermoelectric generators or metalloradiopharmaceuticals.</abstract><cop>Germany</cop><pub>Wiley Blackwell (John Wiley & Sons)</pub><orcidid>https://orcid.org/0000000222191253</orcidid><orcidid>https://orcid.org/0000000245570870</orcidid><orcidid>https://orcid.org/0000000180241661</orcidid><orcidid>https://orcid.org/0000000339734207</orcidid><orcidid>https://orcid.org/0000000227678343</orcidid><orcidid>https://orcid.org/0000000339521949</orcidid><orcidid>https://orcid.org/000000033804487X</orcidid><orcidid>https://orcid.org/0000000277746535</orcidid></addata></record> |
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| title | f‐ block MOFs: A Pathway to Heterometallic Transuranics |
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