Amplifying the Sensitivity of Zinc(II) Responsive MRI Contrast Agents by Altering Water Exchange Rates
Given the known water exchange rate limitations of a previously reported Zn(II)-sensitive MRI contrast agent, GdDOTA-diBPEN, new structural targets were rationally designed to increase the rate of water exchange to improve MRI detection sensitivity. These new sensors exhibit fine-tuned water exchan...
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| Veröffentlicht in: | Journal of the American Chemical Society 2015-11, Vol.137 (44), p.14173-14179 |
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| container_title | Journal of the American Chemical Society |
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| creator | Yu, Jing Martins, André F Preihs, Christian Clavijo Jordan, Veronica Chirayil, Sara Zhao, Piyu Wu, Yunkou Nasr, Khaled Kiefer, Garry E Sherry, A. Dean |
| description | Given the known water exchange rate limitations of a previously reported Zn(II)-sensitive MRI contrast agent, GdDOTA-diBPEN, new structural targets were rationally designed to increase the rate of water exchange to improve MRI detection sensitivity. These new sensors exhibit fine-tuned water exchange properties and, depending on the individual structure, demonstrate significantly improved longitudinal relaxivities (r 1). Two sensors in particular demonstrate optimized parameters and, therefore, show exceptionally high longitudinal relaxivities of about 50 mM–1 s–1 upon binding to Zn(II) and human serum albumin (HSA). This value demonstrates a 3-fold increase in r 1 compared to that displayed by the original sensor, GdDOTA-diBPEN. In addition, this study provides important insights into the interplay between structural modifications, water exchange rate, and kinetic stability properties of the sensors. The new high relaxivity agents were used to successfully image Zn(II) release from the mouse pancreas in vivo during glucose stimulated insulin secretion. |
| doi_str_mv | 10.1021/jacs.5b09158 |
| format | Article |
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Dean</creator><creatorcontrib>Yu, Jing ; Martins, André F ; Preihs, Christian ; Clavijo Jordan, Veronica ; Chirayil, Sara ; Zhao, Piyu ; Wu, Yunkou ; Nasr, Khaled ; Kiefer, Garry E ; Sherry, A. Dean</creatorcontrib><description>Given the known water exchange rate limitations of a previously reported Zn(II)-sensitive MRI contrast agent, GdDOTA-diBPEN, new structural targets were rationally designed to increase the rate of water exchange to improve MRI detection sensitivity. These new sensors exhibit fine-tuned water exchange properties and, depending on the individual structure, demonstrate significantly improved longitudinal relaxivities (r 1). Two sensors in particular demonstrate optimized parameters and, therefore, show exceptionally high longitudinal relaxivities of about 50 mM–1 s–1 upon binding to Zn(II) and human serum albumin (HSA). This value demonstrates a 3-fold increase in r 1 compared to that displayed by the original sensor, GdDOTA-diBPEN. In addition, this study provides important insights into the interplay between structural modifications, water exchange rate, and kinetic stability properties of the sensors. The new high relaxivity agents were used to successfully image Zn(II) release from the mouse pancreas in vivo during glucose stimulated insulin secretion.</description><identifier>ISSN: 0002-7863</identifier><identifier>ISSN: 1520-5126</identifier><identifier>EISSN: 1520-5126</identifier><identifier>DOI: 10.1021/jacs.5b09158</identifier><identifier>PMID: 26462412</identifier><language>eng</language><publisher>United States: American Chemical Society</publisher><subject>Animals ; Contrast Media - chemical synthesis ; Contrast Media - chemistry ; Contrast Media - metabolism ; Coordination Complexes - chemical synthesis ; Coordination Complexes - chemistry ; Coordination Complexes - metabolism ; detection limit ; glucose ; Glucose - chemistry ; Glucose - metabolism ; Heterocyclic Compounds, 1-Ring - chemical synthesis ; Heterocyclic Compounds, 1-Ring - chemistry ; Heterocyclic Compounds, 1-Ring - metabolism ; human serum albumin ; Humans ; Insulin - chemistry ; Insulin - metabolism ; insulin secretion ; Kinetics ; Magnetic Resonance Imaging ; Mice ; Mice, Inbred C57BL ; Molecular Structure ; pancreas ; Pancreas - chemistry ; Pancreas - cytology ; Pancreas - metabolism ; Serum Albumin - chemistry ; Serum Albumin - metabolism ; Thermodynamics ; Water - chemistry ; Water - metabolism ; zinc ; Zinc - chemistry ; Zinc - metabolism</subject><ispartof>Journal of the American Chemical Society, 2015-11, Vol.137 (44), p.14173-14179</ispartof><rights>Copyright © 2015 American Chemical Society</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a450t-2115707483028395dd663fd53cf42c2753a063e84e8c197b48b298898c41ec883</citedby><cites>FETCH-LOGICAL-a450t-2115707483028395dd663fd53cf42c2753a063e84e8c197b48b298898c41ec883</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://pubs.acs.org/doi/pdf/10.1021/jacs.5b09158$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/jacs.5b09158$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>230,314,776,780,881,2751,27055,27903,27904,56716,56766</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/26462412$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Yu, Jing</creatorcontrib><creatorcontrib>Martins, André F</creatorcontrib><creatorcontrib>Preihs, Christian</creatorcontrib><creatorcontrib>Clavijo Jordan, Veronica</creatorcontrib><creatorcontrib>Chirayil, Sara</creatorcontrib><creatorcontrib>Zhao, Piyu</creatorcontrib><creatorcontrib>Wu, Yunkou</creatorcontrib><creatorcontrib>Nasr, Khaled</creatorcontrib><creatorcontrib>Kiefer, Garry E</creatorcontrib><creatorcontrib>Sherry, A. Dean</creatorcontrib><title>Amplifying the Sensitivity of Zinc(II) Responsive MRI Contrast Agents by Altering Water Exchange Rates</title><title>Journal of the American Chemical Society</title><addtitle>J. Am. Chem. Soc</addtitle><description>Given the known water exchange rate limitations of a previously reported Zn(II)-sensitive MRI contrast agent, GdDOTA-diBPEN, new structural targets were rationally designed to increase the rate of water exchange to improve MRI detection sensitivity. These new sensors exhibit fine-tuned water exchange properties and, depending on the individual structure, demonstrate significantly improved longitudinal relaxivities (r 1). Two sensors in particular demonstrate optimized parameters and, therefore, show exceptionally high longitudinal relaxivities of about 50 mM–1 s–1 upon binding to Zn(II) and human serum albumin (HSA). This value demonstrates a 3-fold increase in r 1 compared to that displayed by the original sensor, GdDOTA-diBPEN. In addition, this study provides important insights into the interplay between structural modifications, water exchange rate, and kinetic stability properties of the sensors. The new high relaxivity agents were used to successfully image Zn(II) release from the mouse pancreas in vivo during glucose stimulated insulin secretion.</description><subject>Animals</subject><subject>Contrast Media - chemical synthesis</subject><subject>Contrast Media - chemistry</subject><subject>Contrast Media - metabolism</subject><subject>Coordination Complexes - chemical synthesis</subject><subject>Coordination Complexes - chemistry</subject><subject>Coordination Complexes - metabolism</subject><subject>detection limit</subject><subject>glucose</subject><subject>Glucose - chemistry</subject><subject>Glucose - metabolism</subject><subject>Heterocyclic Compounds, 1-Ring - chemical synthesis</subject><subject>Heterocyclic Compounds, 1-Ring - chemistry</subject><subject>Heterocyclic Compounds, 1-Ring - metabolism</subject><subject>human serum albumin</subject><subject>Humans</subject><subject>Insulin - chemistry</subject><subject>Insulin - metabolism</subject><subject>insulin secretion</subject><subject>Kinetics</subject><subject>Magnetic Resonance Imaging</subject><subject>Mice</subject><subject>Mice, Inbred C57BL</subject><subject>Molecular Structure</subject><subject>pancreas</subject><subject>Pancreas - chemistry</subject><subject>Pancreas - cytology</subject><subject>Pancreas - metabolism</subject><subject>Serum Albumin - chemistry</subject><subject>Serum Albumin - metabolism</subject><subject>Thermodynamics</subject><subject>Water - chemistry</subject><subject>Water - metabolism</subject><subject>zinc</subject><subject>Zinc - chemistry</subject><subject>Zinc - metabolism</subject><issn>0002-7863</issn><issn>1520-5126</issn><issn>1520-5126</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2015</creationdate><recordtype>article</recordtype><sourceid>EIF</sourceid><recordid>eNqFkd-LEzEQx4MoXj1981nyeIJ75vdmX4RSTq9wx0FVBF9CNp1tU7ZJ3aTF_vdmud6pIPg0GeY7n5nMF6HXlFxSwuj7jXXpUrakoVI_QRMqGakkZeopmhBCWFVrxc_Qi5Q2JRVM0-fojCmhmKBsgrrpdtf77ujDCuc14M8Qks_-4PMRxw5_98FdzOdv8QLSLpbSAfDtYo5nMeTBpoynKwg54faIp32GYcR8s-WBr366tQ0rwIuSppfoWWf7BK9O8Rx9_Xj1ZXZd3dx9ms-mN5UVkuSKUSprUgvNCdO8kculUrxbSu46wRyrJbdEcdACtKNN3QrdskbrRjtBwWnNz9GHe-5u325h6WBcsze7wW_tcDTRevN3Jfi1WcWDkXWjlFQFcHECDPHHHlI2W58c9L0NEPfJsHJErqTU5L9SWnMmG9UwUaTv7qVuiCkN0D1uRIkZXTSji-bkYpG_-fMXj-IH236PHrs2cT-EctR_s34B0USk1g</recordid><startdate>20151111</startdate><enddate>20151111</enddate><creator>Yu, Jing</creator><creator>Martins, André F</creator><creator>Preihs, Christian</creator><creator>Clavijo Jordan, Veronica</creator><creator>Chirayil, Sara</creator><creator>Zhao, Piyu</creator><creator>Wu, Yunkou</creator><creator>Nasr, Khaled</creator><creator>Kiefer, Garry E</creator><creator>Sherry, A. Dean</creator><general>American Chemical Society</general><scope>CGR</scope><scope>CUY</scope><scope>CVF</scope><scope>ECM</scope><scope>EIF</scope><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7X8</scope><scope>7S9</scope><scope>L.6</scope><scope>5PM</scope></search><sort><creationdate>20151111</creationdate><title>Amplifying the Sensitivity of Zinc(II) Responsive MRI Contrast Agents by Altering Water Exchange Rates</title><author>Yu, Jing ; Martins, André F ; Preihs, Christian ; Clavijo Jordan, Veronica ; Chirayil, Sara ; Zhao, Piyu ; Wu, Yunkou ; Nasr, Khaled ; Kiefer, Garry E ; Sherry, A. Dean</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a450t-2115707483028395dd663fd53cf42c2753a063e84e8c197b48b298898c41ec883</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2015</creationdate><topic>Animals</topic><topic>Contrast Media - chemical synthesis</topic><topic>Contrast Media - chemistry</topic><topic>Contrast Media - metabolism</topic><topic>Coordination Complexes - chemical synthesis</topic><topic>Coordination Complexes - chemistry</topic><topic>Coordination Complexes - metabolism</topic><topic>detection limit</topic><topic>glucose</topic><topic>Glucose - chemistry</topic><topic>Glucose - metabolism</topic><topic>Heterocyclic Compounds, 1-Ring - chemical synthesis</topic><topic>Heterocyclic Compounds, 1-Ring - chemistry</topic><topic>Heterocyclic Compounds, 1-Ring - metabolism</topic><topic>human serum albumin</topic><topic>Humans</topic><topic>Insulin - chemistry</topic><topic>Insulin - metabolism</topic><topic>insulin secretion</topic><topic>Kinetics</topic><topic>Magnetic Resonance Imaging</topic><topic>Mice</topic><topic>Mice, Inbred C57BL</topic><topic>Molecular Structure</topic><topic>pancreas</topic><topic>Pancreas - chemistry</topic><topic>Pancreas - cytology</topic><topic>Pancreas - metabolism</topic><topic>Serum Albumin - chemistry</topic><topic>Serum Albumin - metabolism</topic><topic>Thermodynamics</topic><topic>Water - chemistry</topic><topic>Water - metabolism</topic><topic>zinc</topic><topic>Zinc - chemistry</topic><topic>Zinc - metabolism</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Yu, Jing</creatorcontrib><creatorcontrib>Martins, André F</creatorcontrib><creatorcontrib>Preihs, Christian</creatorcontrib><creatorcontrib>Clavijo Jordan, Veronica</creatorcontrib><creatorcontrib>Chirayil, Sara</creatorcontrib><creatorcontrib>Zhao, Piyu</creatorcontrib><creatorcontrib>Wu, Yunkou</creatorcontrib><creatorcontrib>Nasr, Khaled</creatorcontrib><creatorcontrib>Kiefer, Garry E</creatorcontrib><creatorcontrib>Sherry, A. 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Dean</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Amplifying the Sensitivity of Zinc(II) Responsive MRI Contrast Agents by Altering Water Exchange Rates</atitle><jtitle>Journal of the American Chemical Society</jtitle><addtitle>J. Am. Chem. Soc</addtitle><date>2015-11-11</date><risdate>2015</risdate><volume>137</volume><issue>44</issue><spage>14173</spage><epage>14179</epage><pages>14173-14179</pages><issn>0002-7863</issn><issn>1520-5126</issn><eissn>1520-5126</eissn><abstract>Given the known water exchange rate limitations of a previously reported Zn(II)-sensitive MRI contrast agent, GdDOTA-diBPEN, new structural targets were rationally designed to increase the rate of water exchange to improve MRI detection sensitivity. These new sensors exhibit fine-tuned water exchange properties and, depending on the individual structure, demonstrate significantly improved longitudinal relaxivities (r 1). Two sensors in particular demonstrate optimized parameters and, therefore, show exceptionally high longitudinal relaxivities of about 50 mM–1 s–1 upon binding to Zn(II) and human serum albumin (HSA). This value demonstrates a 3-fold increase in r 1 compared to that displayed by the original sensor, GdDOTA-diBPEN. In addition, this study provides important insights into the interplay between structural modifications, water exchange rate, and kinetic stability properties of the sensors. The new high relaxivity agents were used to successfully image Zn(II) release from the mouse pancreas in vivo during glucose stimulated insulin secretion.</abstract><cop>United States</cop><pub>American Chemical Society</pub><pmid>26462412</pmid><doi>10.1021/jacs.5b09158</doi><tpages>7</tpages><oa>free_for_read</oa></addata></record> |
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| source | MEDLINE; American Chemical Society Journals |
| subjects | Animals Contrast Media - chemical synthesis Contrast Media - chemistry Contrast Media - metabolism Coordination Complexes - chemical synthesis Coordination Complexes - chemistry Coordination Complexes - metabolism detection limit glucose Glucose - chemistry Glucose - metabolism Heterocyclic Compounds, 1-Ring - chemical synthesis Heterocyclic Compounds, 1-Ring - chemistry Heterocyclic Compounds, 1-Ring - metabolism human serum albumin Humans Insulin - chemistry Insulin - metabolism insulin secretion Kinetics Magnetic Resonance Imaging Mice Mice, Inbred C57BL Molecular Structure pancreas Pancreas - chemistry Pancreas - cytology Pancreas - metabolism Serum Albumin - chemistry Serum Albumin - metabolism Thermodynamics Water - chemistry Water - metabolism zinc Zinc - chemistry Zinc - metabolism |
| title | Amplifying the Sensitivity of Zinc(II) Responsive MRI Contrast Agents by Altering Water Exchange Rates |
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