TmDOTA-Tetraglycinate Encapsulated Liposomes as pH-Sensitive LipoCEST Agents
Identifieur interne : 000392 ( Pmc/Curation ); précédent : 000391; suivant : 000393TmDOTA-Tetraglycinate Encapsulated Liposomes as pH-Sensitive LipoCEST Agents
Auteurs : Ana Christina L. Opina [États-Unis] ; Ketan B. Ghaghada [États-Unis] ; Piyu Zhao [États-Unis] ; Garry Kiefer [États-Unis] ; Ananth Annapragada [États-Unis] ; A. Dean Sherry [États-Unis]Source :
- PLoS ONE [ 1932-6203 ] ; 2011.
Abstract
Lanthanide DOTA-tetraglycinate (LnDOTA-(gly)4−) complexes contain four magnetically equivalent amide protons that exchange with protons of bulk water. The rate of this base catalyzed exchange process has been measured using chemical exchange saturation transfer (CEST) NMR techniques as a function of solution pH for various paramagnetic LnDOTA-(gly)4− complexes to evaluate the effects of lanthanide ion size on this process. Complexes with Tb(III), Dy(III), Tm(III) and Yb(III) were chosen because these ions induce large hyperfine shifts in all ligand protons, including the exchanging amide protons. The magnitude of the amide proton CEST exchange signal differed for the four paramagnetic complexes in order, Yb>Tm>Tb>Dy. Although the Dy(III) complex showed the largest hyperfine shift as expected, the combination of favorable chemical shift and amide proton CEST linewidth in the Tm(III) complex was deemed most favorable for future
Url:
DOI: 10.1371/journal.pone.0027370
PubMed: 22140438
PubMed Central: 3225356
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<sourceDesc><biblStruct><analytic><title xml:lang="en" level="a" type="main">TmDOTA-Tetraglycinate Encapsulated Liposomes as pH-Sensitive LipoCEST Agents</title>
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<author><name sortKey="Zhao, Piyu" sort="Zhao, Piyu" uniqKey="Zhao P" first="Piyu" last="Zhao">Piyu Zhao</name>
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<front><div type="abstract" xml:lang="en"><p>Lanthanide DOTA-tetraglycinate (LnDOTA-(gly)<sub>4</sub>
<sup>−</sup>
) complexes contain four magnetically equivalent amide protons that exchange with protons of bulk water. The rate of this base catalyzed exchange process has been measured using chemical exchange saturation transfer (CEST) NMR techniques as a function of solution pH for various paramagnetic LnDOTA-(gly)<sub>4</sub>
<sup>−</sup>
complexes to evaluate the effects of lanthanide ion size on this process. Complexes with Tb(III), Dy(III), Tm(III) and Yb(III) were chosen because these ions induce large hyperfine shifts in all ligand protons, including the exchanging amide protons. The magnitude of the amide proton CEST exchange signal differed for the four paramagnetic complexes in order, Yb>Tm>Tb>Dy. Although the Dy(III) complex showed the largest hyperfine shift as expected, the combination of favorable chemical shift and amide proton CEST linewidth in the Tm(III) complex was deemed most favorable for future <italic>in vivo</italic>
applications where tissue magnetization effects can interfere. TmDOTA-(gly)<sub>4</sub>
<sup>−</sup>
at various concentrations was encapsulated in the core interior of liposomes to yield lipoCEST particles for molecular imaging. The resulting nanoparticles showed less than 1% leakage of the agent from the interior over a range of temperatures and pH. The pH <italic>versus</italic>
amide proton CEST curves differed for the free <italic>versus</italic>
encapsulated agents over the acidic pH regions, consistent with a lower proton permeability across the liposomal bilayer for the encapsulated agent. Nevertheless, the resulting lipoCEST nanoparticles amplify the CEST sensitivity by a factor of ∼10<sup>4</sup>
compared to the free, un-encapsulated agent. Such pH sensitive nano-probes could prove useful for pH mapping of liposomes targeted to tumors.</p>
</div>
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<front><journal-meta><journal-id journal-id-type="nlm-ta">PLoS One</journal-id>
<journal-id journal-id-type="publisher-id">plos</journal-id>
<journal-id journal-id-type="pmc">plosone</journal-id>
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<publisher><publisher-name>Public Library of Science</publisher-name>
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<article-id pub-id-type="pmc">3225356</article-id>
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<article-id pub-id-type="doi">10.1371/journal.pone.0027370</article-id>
<article-categories><subj-group subj-group-type="heading"><subject>Research Article</subject>
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<subj-group subj-group-type="Discipline-v2"><subject>Chemistry</subject>
<subj-group><subject>Applied Chemistry</subject>
<subj-group><subject>Chemical Properties</subject>
<subj-group><subject>Nuclear Magnetic Resonance</subject>
</subj-group>
</subj-group>
</subj-group>
<subj-group><subject>Inorganic Chemistry</subject>
<subj-group><subject>Inorganic Compounds</subject>
<subj-group><subject>Coordination Compounds</subject>
</subj-group>
</subj-group>
</subj-group>
</subj-group>
<subj-group subj-group-type="Discipline-v2"><subject>Engineering</subject>
<subj-group><subject>Mechanical Engineering</subject>
<subj-group><subject>Nanoengineering</subject>
</subj-group>
</subj-group>
</subj-group>
<subj-group subj-group-type="Discipline-v2"><subject>Materials Science</subject>
<subj-group><subject>Material by Attribute</subject>
<subj-group><subject>Nanomaterials</subject>
</subj-group>
</subj-group>
<subj-group><subject>Nanotechnology</subject>
<subj-group><subject>Nanomaterials</subject>
</subj-group>
</subj-group>
</subj-group>
</article-categories>
<title-group><article-title>TmDOTA-Tetraglycinate Encapsulated Liposomes as pH-Sensitive LipoCEST Agents</article-title>
<alt-title alt-title-type="running-head">pH-Sensitive LipoCEST Agents for MRI</alt-title>
</title-group>
<contrib-group><contrib contrib-type="author"><name><surname>Opina</surname>
<given-names>Ana Christina L.</given-names>
</name>
<xref ref-type="aff" rid="aff1"><sup>1</sup>
</xref>
</contrib>
<contrib contrib-type="author"><name><surname>Ghaghada</surname>
<given-names>Ketan B.</given-names>
</name>
<xref ref-type="aff" rid="aff2"><sup>2</sup>
</xref>
</contrib>
<contrib contrib-type="author"><name><surname>Zhao</surname>
<given-names>Piyu</given-names>
</name>
<xref ref-type="aff" rid="aff1"><sup>1</sup>
</xref>
</contrib>
<contrib contrib-type="author"><name><surname>Kiefer</surname>
<given-names>Garry</given-names>
</name>
<xref ref-type="aff" rid="aff1"><sup>1</sup>
</xref>
</contrib>
<contrib contrib-type="author"><name><surname>Annapragada</surname>
<given-names>Ananth</given-names>
</name>
<xref ref-type="aff" rid="aff2"><sup>2</sup>
</xref>
</contrib>
<contrib contrib-type="author"><name><surname>Sherry</surname>
<given-names>A. Dean</given-names>
</name>
<xref ref-type="aff" rid="aff1"><sup>1</sup>
</xref>
<xref ref-type="aff" rid="aff3"><sup>3</sup>
</xref>
<xref ref-type="corresp" rid="cor1"><sup>*</sup>
</xref>
</contrib>
</contrib-group>
<aff id="aff1"><label>1</label>
<addr-line>Department of Chemistry, University of Texas at Dallas, Richardson, Texas, United States of America</addr-line>
</aff>
<aff id="aff2"><label>2</label>
<addr-line>School of Biomedical Informatics, University of Texas Health Sciences Center at Houston, Houston, Texas, United States of America</addr-line>
</aff>
<aff id="aff3"><label>3</label>
<addr-line>Advanced Imaging Research Center, University of Texas Southwestern Medical Center, Dallas, Texas, United States of America</addr-line>
</aff>
<contrib-group><contrib contrib-type="editor"><name><surname>Brechbiel</surname>
<given-names>Martin W.</given-names>
</name>
<role>Editor</role>
<xref ref-type="aff" rid="edit1"></xref>
</contrib>
</contrib-group>
<aff id="edit1">National Institutes of Health, United States of America</aff>
<author-notes><corresp id="cor1">* E-mail: <email>sherry@utdallas.edu</email>
</corresp>
<fn fn-type="con"><p>Conceived and designed the experiments: ACLO ADS. Performed the experiments: ACLO PZ. Analyzed the data: ACLO KBG AA GK ADS. Contributed reagents/materials/analysis tools: KBG AA. Wrote the paper: ACLO KBG AA ADS.</p>
</fn>
</author-notes>
<pub-date pub-type="collection"><year>2011</year>
</pub-date>
<pub-date pub-type="epub"><day>28</day>
<month>11</month>
<year>2011</year>
</pub-date>
<volume>6</volume>
<issue>11</issue>
<elocation-id>e27370</elocation-id>
<history><date date-type="received"><day>22</day>
<month>6</month>
<year>2011</year>
</date>
<date date-type="accepted"><day>15</day>
<month>10</month>
<year>2011</year>
</date>
</history>
<permissions><copyright-statement>Opina et al. This is an open-access article distributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited.</copyright-statement>
<copyright-year>2011</copyright-year>
</permissions>
<abstract><p>Lanthanide DOTA-tetraglycinate (LnDOTA-(gly)<sub>4</sub>
<sup>−</sup>
) complexes contain four magnetically equivalent amide protons that exchange with protons of bulk water. The rate of this base catalyzed exchange process has been measured using chemical exchange saturation transfer (CEST) NMR techniques as a function of solution pH for various paramagnetic LnDOTA-(gly)<sub>4</sub>
<sup>−</sup>
complexes to evaluate the effects of lanthanide ion size on this process. Complexes with Tb(III), Dy(III), Tm(III) and Yb(III) were chosen because these ions induce large hyperfine shifts in all ligand protons, including the exchanging amide protons. The magnitude of the amide proton CEST exchange signal differed for the four paramagnetic complexes in order, Yb>Tm>Tb>Dy. Although the Dy(III) complex showed the largest hyperfine shift as expected, the combination of favorable chemical shift and amide proton CEST linewidth in the Tm(III) complex was deemed most favorable for future <italic>in vivo</italic>
applications where tissue magnetization effects can interfere. TmDOTA-(gly)<sub>4</sub>
<sup>−</sup>
at various concentrations was encapsulated in the core interior of liposomes to yield lipoCEST particles for molecular imaging. The resulting nanoparticles showed less than 1% leakage of the agent from the interior over a range of temperatures and pH. The pH <italic>versus</italic>
amide proton CEST curves differed for the free <italic>versus</italic>
encapsulated agents over the acidic pH regions, consistent with a lower proton permeability across the liposomal bilayer for the encapsulated agent. Nevertheless, the resulting lipoCEST nanoparticles amplify the CEST sensitivity by a factor of ∼10<sup>4</sup>
compared to the free, un-encapsulated agent. Such pH sensitive nano-probes could prove useful for pH mapping of liposomes targeted to tumors.</p>
</abstract>
<counts><page-count count="10"></page-count>
</counts>
</article-meta>
</front>
</pmc>
</record>
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