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Title: Synthesis and characterization of polylactide-PAMAM “Janus-type” linear-dendritic hybrids

Abstract

In this report, we introduce a facile and comprehensive synthetic methodology for the preparation of polyester-polyamidoamine (PAMAM) (i.e., polyester: polylactide [PLA] (hydrophobic) and polyamidoamine, PAMAM [hydrophilic]) polymers. A library of PLA-PAMAM linear dendritic block copolymers (LDBCs) in which both l and d, l polylactide were employed in mass ratios of 30:70, 50:50, 70:30, and 90:10 (PLA:PAMAM) were synthesized and analyzed. When placed in aqueous media, the immiscibility of the hydrophilic and hydrophobic segments leads to nanophase-segregation exhibited as the formation of aggregates (e.g., vesicles, worms, and/or micelles). By employing both stereochemical configurations of PLA, the differentiation in mass ratios of PLA-PAMAM aided in elucidating the structure–property relationships of the LDBC system and provided a means toward the control of nanoparticle morphology. Transmission electron microscopy and dynamic light scattering afford the size and shape of the nanoparticles with diameters ranging from 10.6 for low mass ratios to 122.4 nm for high mass ratios of PLA-PAMAM and positive zeta-potential values between +24 mV and +48.2 mV. Moreover, small-angle X-ray scattering (SAXS) studies were employed to obtain more detailed information on the morphological assemblies constructed via direct dissolution. Such insights provide a pathway toward nanomaterials with unique morphologies and tunable properties deemed relevantmore » in the development of next generation biomaterials.« less

Authors:
 [1];  [1];  [2];  [1];  [1];  [1];  [1];  [2];  [3];  [1];  [1];  [4];  [3];  [2]; ORCiD logo [1]
  1. Univ. of Mississippi, Oxford, MS (United States)
  2. Louisiana State Univ., Baton Rouge, LA (United States)
  3. Tulane Univ., New Orleans, LA (United States)
  4. Argonne National Lab. (ANL), Lemont, IL (United States)
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); Experimental Program to Stimulate Competitive Research (EPSCoR); Northwestern Univ.; Materials Research Science and Engineering Center (NU-MRSEC); National Science Foundation (NSF)
OSTI Identifier:
1559534
Alternate Identifier(s):
OSTI ID: 1514742
Grant/Contract Number:  
AC02-06CH11357; SC0012432
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Polymer Science. Part A, Polymer Chemistry
Additional Journal Information:
Journal Volume: 57; Journal Issue: 13; Journal ID: ISSN 0887-624X
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; amphiphiles; block copolymers; drug delivery systems; nanoparticles; self‐assembly

Citation Formats

Chandrasiri, Indika, Abebe, Daniel G., Gupta, Sudipta, Williams, Jon Steven Dal, Rieger, William D., Simms, Briana L., Yaddehige, Mahesh Loku, Noh, YeRim, Payne, Molly E., Fortenberry, Alexander W., Smith, Adam E., Ilavsky, Jan, Grayson, Scott M., Schneider, Gerald J., and Watkins, Davita L. Synthesis and characterization of polylactide-PAMAM “Janus-type” linear-dendritic hybrids. United States: N. p., 2019. Web. doi:10.1002/pola.29409.
Chandrasiri, Indika, Abebe, Daniel G., Gupta, Sudipta, Williams, Jon Steven Dal, Rieger, William D., Simms, Briana L., Yaddehige, Mahesh Loku, Noh, YeRim, Payne, Molly E., Fortenberry, Alexander W., Smith, Adam E., Ilavsky, Jan, Grayson, Scott M., Schneider, Gerald J., & Watkins, Davita L. Synthesis and characterization of polylactide-PAMAM “Janus-type” linear-dendritic hybrids. United States. https://doi.org/10.1002/pola.29409
Chandrasiri, Indika, Abebe, Daniel G., Gupta, Sudipta, Williams, Jon Steven Dal, Rieger, William D., Simms, Briana L., Yaddehige, Mahesh Loku, Noh, YeRim, Payne, Molly E., Fortenberry, Alexander W., Smith, Adam E., Ilavsky, Jan, Grayson, Scott M., Schneider, Gerald J., and Watkins, Davita L. Mon . "Synthesis and characterization of polylactide-PAMAM “Janus-type” linear-dendritic hybrids". United States. https://doi.org/10.1002/pola.29409. https://www.osti.gov/servlets/purl/1559534.
@article{osti_1559534,
title = {Synthesis and characterization of polylactide-PAMAM “Janus-type” linear-dendritic hybrids},
author = {Chandrasiri, Indika and Abebe, Daniel G. and Gupta, Sudipta and Williams, Jon Steven Dal and Rieger, William D. and Simms, Briana L. and Yaddehige, Mahesh Loku and Noh, YeRim and Payne, Molly E. and Fortenberry, Alexander W. and Smith, Adam E. and Ilavsky, Jan and Grayson, Scott M. and Schneider, Gerald J. and Watkins, Davita L.},
abstractNote = {In this report, we introduce a facile and comprehensive synthetic methodology for the preparation of polyester-polyamidoamine (PAMAM) (i.e., polyester: polylactide [PLA] (hydrophobic) and polyamidoamine, PAMAM [hydrophilic]) polymers. A library of PLA-PAMAM linear dendritic block copolymers (LDBCs) in which both l and d, l polylactide were employed in mass ratios of 30:70, 50:50, 70:30, and 90:10 (PLA:PAMAM) were synthesized and analyzed. When placed in aqueous media, the immiscibility of the hydrophilic and hydrophobic segments leads to nanophase-segregation exhibited as the formation of aggregates (e.g., vesicles, worms, and/or micelles). By employing both stereochemical configurations of PLA, the differentiation in mass ratios of PLA-PAMAM aided in elucidating the structure–property relationships of the LDBC system and provided a means toward the control of nanoparticle morphology. Transmission electron microscopy and dynamic light scattering afford the size and shape of the nanoparticles with diameters ranging from 10.6 for low mass ratios to 122.4 nm for high mass ratios of PLA-PAMAM and positive zeta-potential values between +24 mV and +48.2 mV. Moreover, small-angle X-ray scattering (SAXS) studies were employed to obtain more detailed information on the morphological assemblies constructed via direct dissolution. Such insights provide a pathway toward nanomaterials with unique morphologies and tunable properties deemed relevant in the development of next generation biomaterials.},
doi = {10.1002/pola.29409},
journal = {Journal of Polymer Science. Part A, Polymer Chemistry},
number = 13,
volume = 57,
place = {United States},
year = {Mon May 20 00:00:00 EDT 2019},
month = {Mon May 20 00:00:00 EDT 2019}
}

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