Unexpected Changes in Functionality and Surface Coverage for Au Nanoparticle PEI Conjugates : Implications for Stability and Efficacy in Biological Systems

Cationic polyethylenimine conjugated gold nanoparticles (AuNP-PEI) are a widely studied vector for drug delivery and an effective probe for interrogating NP-cell interactions. However, an inconsistent body of literature currently exists regarding the reproducibility of physicochemical properties, co...

Ausführliche Beschreibung

Bibliographische Detailangaben
Veröffentlicht in:Langmuir : the ACS journal of surfaces and colloids. - 1985. - 31(2015), 27 vom: 14. Juli, Seite 7673-83
1. Verfasser: Cho, Tae Joon (VerfasserIn)
Weitere Verfasser: Pettibone, John M, Gorham, Justin M, Nguyen, Thao M, MacCuspie, Robert I, Gigault, Julien, Hackley, Vincent A
Format: Online-Aufsatz
Sprache:English
Veröffentlicht: 2015
Zugriff auf das übergeordnete Werk:Langmuir : the ACS journal of surfaces and colloids
Schlagworte:Journal Article Colloids Gold 7440-57-5 Polyethyleneimine 9002-98-6
LEADER 01000caa a22002652c 4500
001 NLM250342960
003 DE-627
005 20250218175529.0
007 cr uuu---uuuuu
008 231224s2015 xx |||||o 00| ||eng c
024 7 |a 10.1021/acs.langmuir.5b01634  |2 doi 
028 5 2 |a pubmed25n0834.xml 
035 |a (DE-627)NLM250342960 
035 |a (NLM)26114747 
040 |a DE-627  |b ger  |c DE-627  |e rakwb 
041 |a eng 
100 1 |a Cho, Tae Joon  |e verfasserin  |4 aut 
245 1 0 |a Unexpected Changes in Functionality and Surface Coverage for Au Nanoparticle PEI Conjugates  |b Implications for Stability and Efficacy in Biological Systems 
264 1 |c 2015 
336 |a Text  |b txt  |2 rdacontent 
337 |a ƒaComputermedien  |b c  |2 rdamedia 
338 |a ƒa Online-Ressource  |b cr  |2 rdacarrier 
500 |a Date Completed 10.05.2016 
500 |a Date Revised 14.07.2015 
500 |a published: Print-Electronic 
500 |a Citation Status MEDLINE 
520 |a Cationic polyethylenimine conjugated gold nanoparticles (AuNP-PEI) are a widely studied vector for drug delivery and an effective probe for interrogating NP-cell interactions. However, an inconsistent body of literature currently exists regarding the reproducibility of physicochemical properties, colloidal stability, and efficacy for these species. To address this gap, we systematically examined the preparation, stability, and formation mechanism of PEI conjugates produced from citrate-capped AuNPs. We considered the dependence on relative molar mass, Mr, backbone conformation, and material source. The conjugation mechanism of Au-PEI was probed using attenuated total reflectance FTIR and X-ray photoelectron spectroscopy, revealing distinct fates for citrate when interacting with different PEI species. The differences in residual citrate, PEI properties, and sample preparation resulted in distinct products with differentiated stability. Overall, branched PEI (25 kDa) conjugates exhibited the greatest colloidal stability in all media tested. By contrast, linear PEI (25 kDa) induced agglomeration. Colloidal stability of the products was also observed to correlate with displaced citrate, which supports a glaring knowledge gap that has emerged regarding the role of this commonly used carboxylate species as a "place holder" for conjugation with ligands of broad functionalities. We observed an unexpected and previously unreported conversion of amine functional groups to quaternary ammonium species for 10 kDa branched conjugates. Results suggest that the AuNP surface catalyzes this conversion. The product is known to manifest distinct processes and uptake in biological systems compared to amines and may lead to unintentional toxicological consequences or decreased efficacy as delivery vectors. Overall, comprehensive physicochemical characterization (tandem spectroscopy methods combined with physical measurements) of the conjugation process provides a methodology for elucidating the contributing factors of colloidal stability and chemical functionality that likely influence the previously reported variations in conjugate properties and biological response models 
650 4 |a Journal Article 
650 7 |a Colloids  |2 NLM 
650 7 |a Gold  |2 NLM 
650 7 |a 7440-57-5  |2 NLM 
650 7 |a Polyethyleneimine  |2 NLM 
650 7 |a 9002-98-6  |2 NLM 
700 1 |a Pettibone, John M  |e verfasserin  |4 aut 
700 1 |a Gorham, Justin M  |e verfasserin  |4 aut 
700 1 |a Nguyen, Thao M  |e verfasserin  |4 aut 
700 1 |a MacCuspie, Robert I  |e verfasserin  |4 aut 
700 1 |a Gigault, Julien  |e verfasserin  |4 aut 
700 1 |a Hackley, Vincent A  |e verfasserin  |4 aut 
773 0 8 |i Enthalten in  |t Langmuir : the ACS journal of surfaces and colloids  |d 1985  |g 31(2015), 27 vom: 14. Juli, Seite 7673-83  |w (DE-627)NLM098181009  |x 1520-5827  |7 nnas 
773 1 8 |g volume:31  |g year:2015  |g number:27  |g day:14  |g month:07  |g pages:7673-83 
856 4 0 |u http://dx.doi.org/10.1021/acs.langmuir.5b01634  |3 Volltext 
912 |a GBV_USEFLAG_A 
912 |a SYSFLAG_A 
912 |a GBV_NLM 
912 |a GBV_ILN_22 
912 |a GBV_ILN_350 
912 |a GBV_ILN_721 
951 |a AR 
952 |d 31  |j 2015  |e 27  |b 14  |c 07  |h 7673-83