Characterization of size, anisotropy, and density heterogeneity of nanoparticles by sedimentation velocity

Handle URI:
http://hdl.handle.net/10754/563691
Title:
Characterization of size, anisotropy, and density heterogeneity of nanoparticles by sedimentation velocity
Authors:
Demeler, Borries; Nguyen, Tich Lam; Gorbet, Gary E.; Schirf, Virgil R.; Brookes, Emre H.; Mulvaney, Paul T.; El-Ballouli, AlA'A O.; Pan, Jun; Bakr, Osman M. ( 0000-0002-3428-1002 ) ; Demeler, Aysha K.; Hernandez Uribe, Blanca I.; Bhattarai, Nabraj; Whetten, Robert L.
Abstract:
A critical problem in materials science is the accurate characterization of the size dependent properties of colloidal inorganic nanocrystals. Due to the intrinsic polydispersity present during synthesis, dispersions of such materials exhibit simultaneous heterogeneity in density ρ, molar mass M, and particle diameter d. The density increments ∂ρ/∂d and ∂ρ/∂M of these nanoparticles, if known, can then provide important information about crystal growth and particle size distributions. For most classes of nanocrystals, a mixture of surfactants is added during synthesis to control their shape, size, and optical properties. However, it remains a challenge to accurately determine the amount of passivating ligand bound to the particle surface post synthesis. The presence of the ligand shell hampers an accurate determination of the nanocrystal diameter. Using CdSe and PbS semiconductor nanocrystals, and the ultrastable silver nanoparticle (M4Ag 44(p-MBA)30), as model systems, we describe a Custom Grid method implemented in UltraScan-III for the characterization of nanoparticles and macromolecules using sedimentation velocity analytical ultracentrifugation. We show that multiple parametrizations are possible, and that the Custom Grid method can be generalized to provide high resolution composition information for mixtures of solutes that are heterogeneous in two out of three parameters. For such cases, our method can simultaneously resolve arbitrary two-dimensional distributions of hydrodynamic parameters when a third property can be held constant. For example, this method extracts partial specific volume and molar mass from sedimentation velocity data for cases where the anisotropy can be held constant, or provides anisotropy and partial specific volume if the molar mass is known. © 2014 American Chemical Society.
KAUST Department:
Physical Sciences and Engineering (PSE) Division; Solar and Photovoltaic Engineering Research Center (SPERC); Materials Science and Engineering Program; Functional Nanomaterials Lab (FuNL)
Publisher:
American Chemical Society (ACS)
Journal:
Analytical Chemistry
Issue Date:
5-Aug-2014
DOI:
10.1021/ac501722r
PubMed ID:
25010012
PubMed Central ID:
PMC4144751
Type:
Article
ISSN:
00032700
Sponsors:
B.D. acknowledges support from the National Science Foundation (Grants ACI-1339649, OCI-1032742, and MCB-070039). O.M.B., A.O.E., and J.P. acknowledge the financial support of KAUST's University Research Fund. P.M. acknowledges support through ARC Grant DP130102134. E.H.B. acknowledges support through NIH/K25GM090154 and NSF/CHE-1265821. B.I.H.U. thanks the trustees of the Max and Minnie Tomerlin Voelcker Fund for financial support through the Voelcker Biomedical Research Academy scholar program. N.B. and R.L.W. acknowledge funding from NSF-PREM DMR-0934218. T.-L.N. thanks Prof. Helmut Colfen from University of Konstanz for the use of the multi-wavelength detected AUC and Mr. Johannes Walter from the Institute of Particle Technology at the University of Erlangen, Germany, for his assistance and the development of the data acquisition software for the multi-wavelength detector used in these experiments.
Additional Links:
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC4144751
Appears in Collections:
Articles; Physical Sciences and Engineering (PSE) Division; Materials Science and Engineering Program; Solar and Photovoltaic Engineering Research Center (SPERC)

Full metadata record

DC FieldValue Language
dc.contributor.authorDemeler, Borriesen
dc.contributor.authorNguyen, Tich Lamen
dc.contributor.authorGorbet, Gary E.en
dc.contributor.authorSchirf, Virgil R.en
dc.contributor.authorBrookes, Emre H.en
dc.contributor.authorMulvaney, Paul T.en
dc.contributor.authorEl-Ballouli, AlA'A O.en
dc.contributor.authorPan, Junen
dc.contributor.authorBakr, Osman M.en
dc.contributor.authorDemeler, Aysha K.en
dc.contributor.authorHernandez Uribe, Blanca I.en
dc.contributor.authorBhattarai, Nabrajen
dc.contributor.authorWhetten, Robert L.en
dc.date.accessioned2015-08-03T12:06:32Zen
dc.date.available2015-08-03T12:06:32Zen
dc.date.issued2014-08-05en
dc.identifier.issn00032700en
dc.identifier.pmid25010012en
dc.identifier.doi10.1021/ac501722ren
dc.identifier.urihttp://hdl.handle.net/10754/563691en
dc.description.abstractA critical problem in materials science is the accurate characterization of the size dependent properties of colloidal inorganic nanocrystals. Due to the intrinsic polydispersity present during synthesis, dispersions of such materials exhibit simultaneous heterogeneity in density ρ, molar mass M, and particle diameter d. The density increments ∂ρ/∂d and ∂ρ/∂M of these nanoparticles, if known, can then provide important information about crystal growth and particle size distributions. For most classes of nanocrystals, a mixture of surfactants is added during synthesis to control their shape, size, and optical properties. However, it remains a challenge to accurately determine the amount of passivating ligand bound to the particle surface post synthesis. The presence of the ligand shell hampers an accurate determination of the nanocrystal diameter. Using CdSe and PbS semiconductor nanocrystals, and the ultrastable silver nanoparticle (M4Ag 44(p-MBA)30), as model systems, we describe a Custom Grid method implemented in UltraScan-III for the characterization of nanoparticles and macromolecules using sedimentation velocity analytical ultracentrifugation. We show that multiple parametrizations are possible, and that the Custom Grid method can be generalized to provide high resolution composition information for mixtures of solutes that are heterogeneous in two out of three parameters. For such cases, our method can simultaneously resolve arbitrary two-dimensional distributions of hydrodynamic parameters when a third property can be held constant. For example, this method extracts partial specific volume and molar mass from sedimentation velocity data for cases where the anisotropy can be held constant, or provides anisotropy and partial specific volume if the molar mass is known. © 2014 American Chemical Society.en
dc.description.sponsorshipB.D. acknowledges support from the National Science Foundation (Grants ACI-1339649, OCI-1032742, and MCB-070039). O.M.B., A.O.E., and J.P. acknowledge the financial support of KAUST's University Research Fund. P.M. acknowledges support through ARC Grant DP130102134. E.H.B. acknowledges support through NIH/K25GM090154 and NSF/CHE-1265821. B.I.H.U. thanks the trustees of the Max and Minnie Tomerlin Voelcker Fund for financial support through the Voelcker Biomedical Research Academy scholar program. N.B. and R.L.W. acknowledge funding from NSF-PREM DMR-0934218. T.-L.N. thanks Prof. Helmut Colfen from University of Konstanz for the use of the multi-wavelength detected AUC and Mr. Johannes Walter from the Institute of Particle Technology at the University of Erlangen, Germany, for his assistance and the development of the data acquisition software for the multi-wavelength detector used in these experiments.en
dc.publisherAmerican Chemical Society (ACS)en
dc.relation.urlhttp://www.ncbi.nlm.nih.gov/pmc/articles/PMC4144751en
dc.titleCharacterization of size, anisotropy, and density heterogeneity of nanoparticles by sedimentation velocityen
dc.typeArticleen
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.contributor.departmentSolar and Photovoltaic Engineering Research Center (SPERC)en
dc.contributor.departmentMaterials Science and Engineering Programen
dc.contributor.departmentFunctional Nanomaterials Lab (FuNL)en
dc.identifier.journalAnalytical Chemistryen
dc.identifier.pmcidPMC4144751en
dc.contributor.institutionDepartment of Biochemistry, University of Texas Health Science Center at San Antonio, 7703 Floyd Curl Drive, San Antonio, TX 78229-3901, United Statesen
dc.contributor.institutionSchool of Chemistry and Bio21 Institute, University of Melbourne, Parkville, VIC 3010, Australiaen
dc.contributor.institutionDepartment of Physics and Astronomy, University of Texas at San Antonio, One UTSA Circle, San Antonio, TX 78249, United Statesen
kaust.authorPan, Junen
kaust.authorBakr, Osman M.en
kaust.authorEl-Ballouli, AlA'A O.en

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