Spittle Stephanie, Poe Derrick, Doherty Brian, Kolodziej Charles, Heroux Luke, Haque Md Ashraful, Squire Henry, Cosby Tyler, Zhang Yong, Fraenza Carla, Bhattacharyya Sahana, Tyagi Madhusudan, Peng Jing, Elgammal Ramez A, Zawodzinski Thomas, Tuckerman Mark, Greenbaum Steve, Gurkan Burcu, Burda Clemens, Dadmun Mark, Maginn Edward J, Sangoro Joshua
Department of Chemical and Biomolecular Engineering, University of Tennessee, Knoxville, TN, 37996, USA.
Department of Chemical and Biomolecular Engineering, University of Notre Dame, Notre Dame, IN, 46556, USA.
Nat Commun. 2022 Jan 11;13(1):219. doi: 10.1038/s41467-021-27842-z.
Deep eutectic solvents (DESs) are an emerging class of non-aqueous solvents that are potentially scalable, easy to prepare and functionalize for many applications ranging from biomass processing to energy storage technologies. Predictive understanding of the fundamental correlations between local structure and macroscopic properties is needed to exploit the large design space and tunability of DESs for specific applications. Here, we employ a range of computational and experimental techniques that span length-scales from molecular to macroscopic and timescales from picoseconds to seconds to study the evolution of structure and dynamics in model DESs, namely Glyceline and Ethaline, starting from the parent compounds. We show that systematic addition of choline chloride leads to microscopic heterogeneities that alter the primary structural relaxation in glycerol and ethylene glycol and result in new dynamic modes that are strongly correlated to the macroscopic properties of the DES formed.
深共熔溶剂（DESs）是一类新兴的非水溶剂，具有潜在的可扩展性，易于制备且可针对从生物质处理到储能技术等许多应用进行功能化。为了利用DESs在特定应用中的巨大设计空间和可调性，需要对局部结构与宏观性质之间的基本相关性有预测性的理解。在此，我们采用一系列从分子到宏观的长度尺度以及从皮秒到秒的时间尺度的计算和实验技术，来研究模型DESs（即甘油和乙二醇）从母体化合物开始的结构和动力学演变。我们表明，氯化胆碱的系统添加会导致微观不均匀性，从而改变甘油和乙二醇中的主要结构弛豫，并产生与所形成的DES的宏观性质密切相关的新动态模式。
