Coacervation of oppositely charged macromolecules, micelles and proteins: Disproportionation and hierarchical structures
Başlık çevirisi mevcut değil.
- Tez No: 402205
- Danışmanlar: PROF. PAUL L. DUBIN
- Tez Türü: Doktora
- Konular: Kimya, Kimya Mühendisliği, Chemistry, Chemical Engineering
- Anahtar Kelimeler: Belirtilmemiş.
- Yıl: 2014
- Dil: İngilizce
- Üniversite: University of Massachusetts Amherst
- Enstitü: Yurtdışı Enstitü
- Ana Bilim Dalı: Belirtilmemiş.
- Bilim Dalı: Belirtilmemiş.
- Sayfa Sayısı: 215
Özet
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Özet (Çeviri)
Analogous disproportionation processes lead to similarities in the structures present at incipient coacervation to those within the subsequent dense phase. Coacervation in polyelectrolyte/mixed ınicelle systeın is induced by teınperature to explore structural evolution before, during and after coacervation. Assemblies of polyelectrolyte-micelle priınary complexes appear to be governed by the interparticle interaction, a delicate balance between short-range attraction and long-range repulsion. Dilution-induced coacervation in opposite to self-suppression is facilitated by the presence of sınailer particles in size but larger in nuınber as a result of the favourable interparticle interaction. While dilution leads to forınation of sınailer particles that can phase separate easily, larger particles can achieve coacervation by increase in teınperature, a greater entropy contribution. Dynamic light scattering reveals a progressive increase in aggregate size with teınperature up to the phase transition at T9, followed by splitting of these aggregates into respectively sınailer and larger particles. The fact that the process of coacervation itself is accompanied by the expulsion of sınailer aggregates to form near-neutral aggregates is known as a type of ınacroion disproportionation. At incipient coacervation, the transfer aınong soluble complexes of excess ınacroions to achieve near-neutrality is found to be analogous to the expulsion (with counterions) of excess ınacroions into dilute domains in the coacervates. The driving forces of ion-pairing and counterion release, in one-phase and dense phase states, use similar strategies of disproportionation and local charge neutralization to form analogous transient structures. The transient nature of coacervate structure is further investigated by rheology and total internal reflection ınicroscopy in PDADMAC/BSA coacervates. While polyelectrolyte-colloid coacervates exhibit structural rearrangeınent in the coacervate correlated with the compositional di Derence between supernatant and coacervate, heteroprotein coacervation appears to have a fıxed stoichioınetry in both phases. The absence of disproportionation is suggested to be responsible for the highly limited conditions of pH, ionic strength I, total protein concentration C/>, and BLG:LF stoichiometry under which Lactoferrin (LF) and P-lactoglobulin (BLG) form optically clear coacervates. These constraints on conditions for pure coacervation were also attributed to the requirements for the formation of a basic primary unit, LF(BLG)4 , characterized in the supernatant and coacervate. Coacervate is characterized as a solidlike transient network of primary units embedded into a viscoelastic suspending fluid.
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