Liquid-Liquid Phase Separation? Ask the Water!

被引:38
|
作者
Pezzotti, Simone [1 ]
Koenig, Benedikt [1 ]
Ramos, Sashary [1 ]
Schwaab, Gerhard [1 ]
Havenith, Martina [1 ,2 ]
机构
[1] Ruhr Univ Bochum, Dept Phys Chem 2, D-44801 Bochum, Germany
[2] Tech Univ Dortmund, Dept Phys, D-44227 Dortmund, Germany
来源
JOURNAL OF PHYSICAL CHEMISTRY LETTERS | 2023年 / 14卷 / 06期
基金
欧盟地平线“2020”; 欧洲研究理事会;
关键词
HYDRATION-SHELL; HYDROPHOBICITY; INTERFACES; PROTEINS; FUS;
D O I
10.1021/acs.jpclett.2c02697
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Water is more than an inert spectator during liquid-liquid phase separation (LLPS), the reversible compartmentalization of protein solutions into a protein-rich and a dilute phase. We show that LLPS is driven by changes in hydration entropy and enthalpy. Tuning LLPS by adjusting experimental parameters, e.g., addition of co-solutes, is a major goal for biological and medical applications. This requires a general model to quantify thermodynamic driving forces. Here, we develop such a model based on the measured amplitudes of characteristic THz-features of two hydration populations: "Cavity-wrap" water hydrating hydrophobic patches is released during LLPS leading to an increase in entropy. "Bound" water hydrating hydrophilic patches is retained since it is enthalpically favorable. We introduce a THzphase diagram mapping these spectroscopic/thermodynamic changes. This provides not only a precise understanding of hydrophobic and hydrophilic hydration driving forces as a function of temperature and concentration but also a rational means to tune LLPS.
引用
收藏
页码:1556 / 1563
页数:8
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