Theoretical insights on the hydration of quinones as catholytes in aqueous redox flow batteries  

作　　者：Jipeng Li Huan Xu Jingqi Wang Yujun Wang Diannan Lu Jichang Liu Jianzhong Wu 

机构地区：[1]Department of Chemical Engineering,Tsinghua University,Beijing 100084,China [2]State Key Laboratory of Chemical Engineering,School of Chemical Engineering,East China University of Science and Technology,Shanghai 200237,China [3]Department of Chemical and Environmental Engineering and Department of Mathematics,University of California,Riverside,CA 92521,USA

出　　处：《Chinese Journal of Chemical Engineering》2021年第9期72-78,共7页中国化学工程学报（英文版）

基　　金：supported by the National Natural Science Foundation of China(U1862204);the U.S.National Science Foundation(NSF-1940118)。

摘　　要：Quinones have been widely studied as a potential catholyte in water-based redox flow batteries(RFBs)due to their ability to carry both electrons and protons in aqueous solutions.The wide variety of quinones and derivatives offers exciting opportunities to optimize the device performance while poses theoretical challenges to quantify their electrochemical behavior as required for molecular design.Computational screening of target quinones with high performance is far from satisfactory.While solvation of quinones affects their potential application in RFBs in terms of both electrochemical windows,stability,and charge transport,experimental data for the solvation structure and solvation free energies are rarely available if not incomplete.Besides,conventional thermodynamic models are mostly unreliable to estimate the properties of direct interest for electrochemical applications.Here,we analyze the hydration free energies of more than 1,400 quinones by combining the first-principles calculations and the classical density functional theory.In order to attain chemical insights and possible trends,special attention is placed on the effects of"backbones"and functional groups on the solvation behavior.The theoretical results provide a thermodynamic basis for the design,synthesis,and screening of high-performance catholytes for electrical energy storage.

关 键 词：QUINONES Classical density functional theory(cDFT) Quantum mechanics(QM) Water-based redox flow batteries(RFBs) Solubility Solvation free energy 

分 类 号：TM912[电气工程—电力电子与电力传动]