Gated and Near-Surface Diffusion of Charged Fullerenes in Nanochannels
Nanoparticles and their derivatives have engendered significant recent interest. Despite considerable advances in nanofluidic physics, control over nanoparticle diffusive transport, requisite for a host of innovative applications, has yet to be demonstrated. In this study, we performed diffusion exp...
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Veröffentlicht in: | ACS nano 2011-12, Vol.5 (12), p.9382-9391 |
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creator | Grattoni, Alessandro Fine, Daniel Zabre, Erika Ziemys, Arturas Gill, Jaskaran Mackeyev, Yuri Cheney, Matthew A Danila, Delia C Hosali, Sharath Wilson, Lon J Hussain, Fazle Ferrari, Mauro |
description | Nanoparticles and their derivatives have engendered significant recent interest. Despite considerable advances in nanofluidic physics, control over nanoparticle diffusive transport, requisite for a host of innovative applications, has yet to be demonstrated. In this study, we performed diffusion experiments for negatively and positively charged fullerene derivatives (dendritic fullerene-1, DF-1, and amino fullerene, AC60) in 5.7 and 13 nm silicon nanochannels in solutions with different ionic strengths. With DF-1, we demonstrated a gated diffusion whereby precise and reproducible control of the dynamics of the release profile was achieved by tuning the gradient of the ionic strength within the nanochannels. With AC60, we observed a near-surface diffusive transport that produced release rates that were independent of the size of the nanochannels within the range of our experiments. Finally, through theoretical analysis we were able to elucidate the relative importance of physical nanoconfinement, electrostatic interactions, and ionic strength heterogeneity with respect to these gated and near-surface diffusive transport phenomena. These results are significant for multiple applications, including the controlled administration of targeted nanovectors for therapeutics. |
doi_str_mv | 10.1021/nn2037863 |
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Despite considerable advances in nanofluidic physics, control over nanoparticle diffusive transport, requisite for a host of innovative applications, has yet to be demonstrated. In this study, we performed diffusion experiments for negatively and positively charged fullerene derivatives (dendritic fullerene-1, DF-1, and amino fullerene, AC60) in 5.7 and 13 nm silicon nanochannels in solutions with different ionic strengths. With DF-1, we demonstrated a gated diffusion whereby precise and reproducible control of the dynamics of the release profile was achieved by tuning the gradient of the ionic strength within the nanochannels. With AC60, we observed a near-surface diffusive transport that produced release rates that were independent of the size of the nanochannels within the range of our experiments. Finally, through theoretical analysis we were able to elucidate the relative importance of physical nanoconfinement, electrostatic interactions, and ionic strength heterogeneity with respect to these gated and near-surface diffusive transport phenomena. These results are significant for multiple applications, including the controlled administration of targeted nanovectors for therapeutics.</description><identifier>ISSN: 1936-0851</identifier><identifier>EISSN: 1936-086X</identifier><identifier>DOI: 10.1021/nn2037863</identifier><identifier>PMID: 22032773</identifier><language>eng</language><publisher>United States: American Chemical Society</publisher><subject>Charging ; Computer Simulation ; Derivatives ; Diffusion ; Fullerenes ; Fullerenes - chemistry ; Materials Testing ; Models, Chemical ; Models, Molecular ; Nanoparticles ; Nanostructure ; Nanostructures - chemistry ; Nanostructures - ultrastructure ; Porosity ; Static Electricity ; Strength ; Transport ; Tuning</subject><ispartof>ACS nano, 2011-12, Vol.5 (12), p.9382-9391</ispartof><rights>Copyright © 2011 American Chemical Society</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a347t-f7a18f04f0099ad9c0519cae5485b9db7cf75bc27e19d16c8f83ea04bbb5c7823</citedby><cites>FETCH-LOGICAL-a347t-f7a18f04f0099ad9c0519cae5485b9db7cf75bc27e19d16c8f83ea04bbb5c7823</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/nn2037863$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/nn2037863$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>314,776,780,2752,27053,27901,27902,56713,56763</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/22032773$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Grattoni, Alessandro</creatorcontrib><creatorcontrib>Fine, Daniel</creatorcontrib><creatorcontrib>Zabre, Erika</creatorcontrib><creatorcontrib>Ziemys, Arturas</creatorcontrib><creatorcontrib>Gill, Jaskaran</creatorcontrib><creatorcontrib>Mackeyev, Yuri</creatorcontrib><creatorcontrib>Cheney, Matthew A</creatorcontrib><creatorcontrib>Danila, Delia C</creatorcontrib><creatorcontrib>Hosali, Sharath</creatorcontrib><creatorcontrib>Wilson, Lon J</creatorcontrib><creatorcontrib>Hussain, Fazle</creatorcontrib><creatorcontrib>Ferrari, Mauro</creatorcontrib><title>Gated and Near-Surface Diffusion of Charged Fullerenes in Nanochannels</title><title>ACS nano</title><addtitle>ACS Nano</addtitle><description>Nanoparticles and their derivatives have engendered significant recent interest. Despite considerable advances in nanofluidic physics, control over nanoparticle diffusive transport, requisite for a host of innovative applications, has yet to be demonstrated. In this study, we performed diffusion experiments for negatively and positively charged fullerene derivatives (dendritic fullerene-1, DF-1, and amino fullerene, AC60) in 5.7 and 13 nm silicon nanochannels in solutions with different ionic strengths. With DF-1, we demonstrated a gated diffusion whereby precise and reproducible control of the dynamics of the release profile was achieved by tuning the gradient of the ionic strength within the nanochannels. With AC60, we observed a near-surface diffusive transport that produced release rates that were independent of the size of the nanochannels within the range of our experiments. Finally, through theoretical analysis we were able to elucidate the relative importance of physical nanoconfinement, electrostatic interactions, and ionic strength heterogeneity with respect to these gated and near-surface diffusive transport phenomena. These results are significant for multiple applications, including the controlled administration of targeted nanovectors for therapeutics.</description><subject>Charging</subject><subject>Computer Simulation</subject><subject>Derivatives</subject><subject>Diffusion</subject><subject>Fullerenes</subject><subject>Fullerenes - chemistry</subject><subject>Materials Testing</subject><subject>Models, Chemical</subject><subject>Models, Molecular</subject><subject>Nanoparticles</subject><subject>Nanostructure</subject><subject>Nanostructures - chemistry</subject><subject>Nanostructures - ultrastructure</subject><subject>Porosity</subject><subject>Static Electricity</subject><subject>Strength</subject><subject>Transport</subject><subject>Tuning</subject><issn>1936-0851</issn><issn>1936-086X</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2011</creationdate><recordtype>article</recordtype><sourceid>EIF</sourceid><recordid>eNp90L1OwzAUhmELgWj5GbgBlAUBQ8B24tgeUaEFqSoDILFFJ84xTZU6xW4G7h6jlk6I6Zzh0Te8hJwxesMoZ7fOcZpJVWR7ZMh0VqRUFe_7u1-wATkKYUGpkEoWh2TAo-dSZkMynsAa6wRcncwQfPrSewsGk_vG2j40nUs6m4zm4D-iGvdtix4dhqRxyQxcZ-bgHLbhhBxYaAOebu8xeRs_vI4e0-nz5Gl0N00hy-U6tRKYsjS3lGoNtTZUMG0ARa5EpetKGitFZbhEpmtWGGVVhkDzqqqEkYpnx-Rys7vy3WePYV0um2CwbcFh14dSM66ZlIJFefWvZLLgsYeQNNLrDTW-C8GjLVe-WYL_KhktfwKXu8DRnm9n-2qJ9U7-Fo3gYgPAhHLR9d7FHn8MfQNCMYBA</recordid><startdate>20111227</startdate><enddate>20111227</enddate><creator>Grattoni, Alessandro</creator><creator>Fine, Daniel</creator><creator>Zabre, Erika</creator><creator>Ziemys, Arturas</creator><creator>Gill, Jaskaran</creator><creator>Mackeyev, Yuri</creator><creator>Cheney, Matthew A</creator><creator>Danila, Delia C</creator><creator>Hosali, Sharath</creator><creator>Wilson, Lon J</creator><creator>Hussain, Fazle</creator><creator>Ferrari, Mauro</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>7SR</scope><scope>7U5</scope><scope>8BQ</scope><scope>8FD</scope><scope>JG9</scope><scope>L7M</scope><scope>7X8</scope></search><sort><creationdate>20111227</creationdate><title>Gated and Near-Surface Diffusion of Charged Fullerenes in Nanochannels</title><author>Grattoni, Alessandro ; Fine, Daniel ; Zabre, Erika ; Ziemys, Arturas ; Gill, Jaskaran ; Mackeyev, Yuri ; Cheney, Matthew A ; Danila, Delia C ; Hosali, Sharath ; Wilson, Lon J ; Hussain, Fazle ; Ferrari, Mauro</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a347t-f7a18f04f0099ad9c0519cae5485b9db7cf75bc27e19d16c8f83ea04bbb5c7823</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2011</creationdate><topic>Charging</topic><topic>Computer Simulation</topic><topic>Derivatives</topic><topic>Diffusion</topic><topic>Fullerenes</topic><topic>Fullerenes - chemistry</topic><topic>Materials Testing</topic><topic>Models, Chemical</topic><topic>Models, Molecular</topic><topic>Nanoparticles</topic><topic>Nanostructure</topic><topic>Nanostructures - chemistry</topic><topic>Nanostructures - ultrastructure</topic><topic>Porosity</topic><topic>Static Electricity</topic><topic>Strength</topic><topic>Transport</topic><topic>Tuning</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Grattoni, Alessandro</creatorcontrib><creatorcontrib>Fine, Daniel</creatorcontrib><creatorcontrib>Zabre, Erika</creatorcontrib><creatorcontrib>Ziemys, Arturas</creatorcontrib><creatorcontrib>Gill, Jaskaran</creatorcontrib><creatorcontrib>Mackeyev, Yuri</creatorcontrib><creatorcontrib>Cheney, Matthew A</creatorcontrib><creatorcontrib>Danila, Delia C</creatorcontrib><creatorcontrib>Hosali, Sharath</creatorcontrib><creatorcontrib>Wilson, Lon J</creatorcontrib><creatorcontrib>Hussain, Fazle</creatorcontrib><creatorcontrib>Ferrari, Mauro</creatorcontrib><collection>Medline</collection><collection>MEDLINE</collection><collection>MEDLINE (Ovid)</collection><collection>MEDLINE</collection><collection>MEDLINE</collection><collection>PubMed</collection><collection>CrossRef</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><collection>MEDLINE - Academic</collection><jtitle>ACS nano</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Grattoni, Alessandro</au><au>Fine, Daniel</au><au>Zabre, Erika</au><au>Ziemys, Arturas</au><au>Gill, Jaskaran</au><au>Mackeyev, Yuri</au><au>Cheney, Matthew A</au><au>Danila, Delia C</au><au>Hosali, Sharath</au><au>Wilson, Lon J</au><au>Hussain, Fazle</au><au>Ferrari, Mauro</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Gated and Near-Surface Diffusion of Charged Fullerenes in Nanochannels</atitle><jtitle>ACS nano</jtitle><addtitle>ACS Nano</addtitle><date>2011-12-27</date><risdate>2011</risdate><volume>5</volume><issue>12</issue><spage>9382</spage><epage>9391</epage><pages>9382-9391</pages><issn>1936-0851</issn><eissn>1936-086X</eissn><abstract>Nanoparticles and their derivatives have engendered significant recent interest. Despite considerable advances in nanofluidic physics, control over nanoparticle diffusive transport, requisite for a host of innovative applications, has yet to be demonstrated. In this study, we performed diffusion experiments for negatively and positively charged fullerene derivatives (dendritic fullerene-1, DF-1, and amino fullerene, AC60) in 5.7 and 13 nm silicon nanochannels in solutions with different ionic strengths. With DF-1, we demonstrated a gated diffusion whereby precise and reproducible control of the dynamics of the release profile was achieved by tuning the gradient of the ionic strength within the nanochannels. With AC60, we observed a near-surface diffusive transport that produced release rates that were independent of the size of the nanochannels within the range of our experiments. 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subjects | Charging Computer Simulation Derivatives Diffusion Fullerenes Fullerenes - chemistry Materials Testing Models, Chemical Models, Molecular Nanoparticles Nanostructure Nanostructures - chemistry Nanostructures - ultrastructure Porosity Static Electricity Strength Transport Tuning |
title | Gated and Near-Surface Diffusion of Charged Fullerenes in Nanochannels |
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