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Concentration Fluctuations near Lower Critical Solution Temperature in Ternary Aqueous Solutions
Macromolecules ( IF 5.1 ) Pub Date : 2017-09-07 00:00:00 , DOI: 10.1021/acs.macromol.7b01502 Di Jia 1, 2 , Murugappan Muthukumar 3 , He Cheng 1, 2 , Charles C. Han 4 , Boualem Hammouda 5
Macromolecules ( IF 5.1 ) Pub Date : 2017-09-07 00:00:00 , DOI: 10.1021/acs.macromol.7b01502 Di Jia 1, 2 , Murugappan Muthukumar 3 , He Cheng 1, 2 , Charles C. Han 4 , Boualem Hammouda 5
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The effects of osmolytes, such as trimethylamine N-oxide (TMAO), on the phase transition in an aqueous solution of polymer, protein, or DNA are very complex, and several phase transitions can occur. In order to explore such effects, we take a simple ternary system of poly(N,N-diethylacrylamide) and a favorable solvent pair TMAO and water to monitor the reduction in the miscibility of the polymer using small-angle neutron scattering (SANS) and dynamic light scattering (DLS). The result shows that the LCST of PDEA solutions is significantly depressed by TMAO. Although DLS data clearly show that aggregates can form as precursors in the homogeneous one-phase region depending on the TMAO concentration, after removing the low-q aggregate region, the three-component system still obeys the mean-field theory. Based on the ternary random phase approximation (RPA) theory, three Flory–Huggins interaction parameters, i.e., χD2O–TMAO, χPDEA–TMAO, and χPDEA–D2O, are obtained to reveal the microscopic origin of this shift in LCST; that is, the strong TMAO–D2O interaction leads to the decrease of LCST. Our study opens up many directions to explore effects such as the interference between aggregation and microphase separation.
中文翻译：
三元水溶液中较低临界溶液温度附近的浓度波动
渗透剂，例如三甲胺N-氧化物（TMAO），对聚合物，蛋白质或DNA水溶液中的相变的影响非常复杂，可能会发生多个相变。为了探讨这种影响，我们采用了一个简单的三元体系的聚（N，N-二乙基丙烯酰胺）和有利的溶剂对TMAO和水，以使用小角度中子散射（SANS）和动态光散射（DLS）。结果表明，TMAO大大降低了PDEA溶液的LCST。尽管DLS数据清楚地表明，根据TMAO的浓度，去除低q值后，聚集体可以在均匀的一相区域中形成前体。在聚合区域，三分量系统仍然遵循均值场理论。基于该三元随机相位近似（RPA）理论，三弗洛里-赫金斯相互作用参数，即χ d 2 -O-TMAO，χ PDEA-TMAO，和χ PDEA-d 2 ö，得到揭示此微观原点LCST的转变；也就是说，TMAO–D 2 O的强相互作用导致LCST的降低。我们的研究为探索诸如聚集和微相分离之间的干扰等影响开辟了许多方向。
更新日期：2017-09-07
中文翻译：
三元水溶液中较低临界溶液温度附近的浓度波动
渗透剂，例如三甲胺N-氧化物（TMAO），对聚合物，蛋白质或DNA水溶液中的相变的影响非常复杂，可能会发生多个相变。为了探讨这种影响，我们采用了一个简单的三元体系的聚（N，N-二乙基丙烯酰胺）和有利的溶剂对TMAO和水，以使用小角度中子散射（SANS）和动态光散射（DLS）。结果表明，TMAO大大降低了PDEA溶液的LCST。尽管DLS数据清楚地表明，根据TMAO的浓度，去除低q值后，聚集体可以在均匀的一相区域中形成前体。在聚合区域，三分量系统仍然遵循均值场理论。基于该三元随机相位近似（RPA）理论，三弗洛里-赫金斯相互作用参数，即χ d 2 -O-TMAO，χ PDEA-TMAO，和χ PDEA-d 2 ö，得到揭示此微观原点LCST的转变；也就是说，TMAO–D 2 O的强相互作用导致LCST的降低。我们的研究为探索诸如聚集和微相分离之间的干扰等影响开辟了许多方向。
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