Temperature-dependent reentrant phase transition of RNA-polycation mixtures.
Temperature-dependent reentrant phase transition of RNA-polycation mixtures.
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DOI：
10.1039/d1sm01557e
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发表时间：
2022-02-16
期刊：
影响因子：
3.4
通讯作者：
Banerjee PR
中科院分区：
文献类型：
--
作者：
Pullara P;Alshareedah I;Banerjee PR
多价生物聚合物的液液相分离是生物体系中普遍存在的过程，在仿生软物质设计中具有重要意义。生物分子的相行为，如蛋白质和核酸，通常由初级链序列编码，并受溶剂性质调节。温度是LLP最重要的物理调节器之一。蛋白质和/或核酸的溶液已被证明在冷却(具有较高的临界溶液温度，UCST)或加热(具有较低的临界溶液温度，LCST)时经历液-液分离。然而，许多理论框架表明，可能存在更复杂的随温度变化的相行为，例如沙漏相图或同时发生UCST和LCST相变的闭环相图。在这里，我们报告了RNA-多胺混合物经历了随温度变化的重入相分离。具体地说，在低温下，RNA-多胺混合物形成均相。升高温度会导致RNA-多胺缩合物的形成。温度的进一步升高会导致凝析油的溶解，形成可再入的均相。RNA的这种双反应相分离不仅是多胺所特有的，而且也可以在短阳离子多肽中观察到。不混溶间隙由聚阳离子电荷、盐浓度和混合物组成控制。基于已有的复凝聚理论，我们的结果指出了去溶熵、离子对和静电相互作用在决定RNA-聚阳离子混合物的闭环相行为中的复杂相互作用。
Liquid-liquid phase separation (LLPS) of multivalent biopolymers is a ubiquitous process in biological systems and is of importance in bio-mimetic soft matter design. The phase behavior of biomolecules, such as proteins and nucleic acids, is typically encoded by the primary chain sequence and regulated by solvent properties. One of the most important physical modulators of LLPS is temperature. Solutions of proteins and/or nucleic acids have been shown to undergo liquid-liquid phase separation either upon cooling (with an upper critical solution temperature, UCST) or upon heating (with a lower critical solution temperature, LCST). However, many theoretical frameworks suggest the possibility of more complex temperature-dependent phase behaviors, such as an hourglass or a closed-loop phase diagram with concurrent UCST and LCST transitions. Here, we report that RNA-polyamine mixtures undergo a reentrant phase separation with temperature. Specifically, at low temperatures, RNA-polyamine mixtures form a homogenous phase. Increasing the temperature leads to the formation of RNA-polyamine condensates. A further increase in temperature leads to the dissolution of condensates, rendering a reentrant homogenous phase. This dual-response phase separation of RNA is not unique to polyamines but also observed with short cationic peptides. The immiscibility gap is controlled by the charge of the polycation, salt concentration, and mixture composition. Based on the existing theories of complex coacervation, our results point to a complex interplay between desolvation entropy, ion-pairing, and electrostatic interactions in dictating the closed-loop phase behavior of RNA-polycation mixtures.
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影响因子：
16
作者：
Dao TP;Kolaitis RM;Kim HJ;O'Donovan K;Martyniak B;Colicino E;Hehnly H;Taylor JP;Castañeda CA
通讯作者：
Castañeda CA
影响因子：
16.6
作者：
Ambadipudi S;Biernat J;Riedel D;Mandelkow E;Zweckstetter M
通讯作者：
Zweckstetter M
影响因子：
15
作者：
Fu, Jingcheng;Schlenoff, Joseph B.
通讯作者：
Schlenoff, Joseph B.
DOI：
10.1039/df9531500188
发表时间：
1953-01-01
期刊：
DISCUSSIONS OF THE FARADAY SOCIETY
影响因子：
--
作者：
BARKER, JA;FOCK, W
通讯作者：
FOCK, W
影响因子：
16.6
作者：
Fares HM;Marras AE;Ting JM;Tirrell MV;Keating CD
通讯作者：
Keating CD