期刊
LANGMUIR
卷 28, 期 21, 页码 7976-7989出版社
AMER CHEMICAL SOC
DOI: 10.1021/la300266h
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资金
- Swedish Research Council (VR) through the Linnaeus grant Organizing Molecular Matter (OMM) Center of Excellence [239-2009-6794]
- Portuguese Science Council (Fundacao para a Ciencia e a Tecnologia, FCT) [SFRH/BPD/48522/2008]
- FCT
- Fundação para a Ciência e a Tecnologia [SFRH/BPD/48522/2008] Funding Source: FCT
The macroscopic phase behavior and other physicochemical properties of dilute aqueous mixtures of DNA and the cationic surfactant hexadecyltrimethylammounium bromide (CTAB), DNA and the polyamine spermine, or DNA, CTAB, and (2-hydroxypropyl)-beta-cyclodextrin (2HP beta CD) were investigated. When DNA is mixed with CTAB we found, with increasing surfactant concentration, (1) free DNA coexisting with surfactant unimers, (2) free DNA coexisting with aggregates of condensed DNA and CTAB, (3) a miscibility gap where macroscopic phase separation is observed, and (4) positively overcharged aggregates of condensed DNA and CTAB. The presence of a clear solution beyond the miscibility gap cannot be ascribed to self-screening by the charges from the DNA and/or the surfactant; instead, hydrophobic interactions among the surfactants are instrumental for the observed behavior. It is difficult to judge whether the overcharged mixed aggregates represent an equilibrium situation or not. If the excess surfactant was not initially present, but added to a preformed precipitate, redissolution was, in consistency with previous reports, not observed; thus, kinetic effects have major influence on the behavior. Mixtures of DNA and spermine also displayed a miscibility gap; however, positively overcharged aggregates were not identified, and redissolution with excess spermine can be explained by electrostatics. When 2HP beta CD was added to a DNA-CTAB precipitate, redissolution was observed, and when it was added to the overcharged aggregates, the behavior was essentially a reversal of that of the DNA-CTAB system. This is attributed to an effectively quantitative formation of 1:1 2HP beta CD-surfactant inclusion complexes, which results in a gradual decrease in the concentration of effectively available surfactant with increasing 2HP beta CD concentration.
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