使用高通量机器学习和理论计算的氧化还原液电池醌电解质的计算设计

IF 2.5 Q3 BIOTECHNOLOGY & APPLIED MICROBIOLOGY
Fei Wang, Jipeng Li, Zheng Liu, Tong Qiu, Jianzhong Wu, Diannan Lu
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引用次数: 1

摘要

具有更高溶解度和更大氧化还原电位窗口的氧化还原活性材料的分子设计有助于提高氧化还原液流电池的性能。本文提出了一种结合机器学习、量子力学和经典密度泛函理论计算的有机氧化还原活性物质的系统评估计算程序。以不同取代基的苯醌、萘醌和蒽醌为基础,合成了1517个小醌分子。基于物理的方法分别预测了HOMO-LUMO间隙和溶剂化自由能,它们分别解释了氧化还原电位差和水溶解度。通过定量结构-性能关系分析和机器学习/图网络建模来评估材料的整体行为,增加了高通量计算。该计算程序能够重现与实验观察一致的高性能阴极电解质材料,并通过筛选100,000个二取代醌分子(迄今为止研究过的最大的氧化还原活性醌分子库)来确定RFBs的新电解质。这一高效的计算平台有助于更好地理解醌类分子的结构-功能关系,促进rfb全有机活性材料的设计和应用。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Computational design of quinone electrolytes for redox flow batteries using high-throughput machine learning and theoretical calculations
Molecular design of redox-active materials with higher solubility and greater redox potential windows is instrumental in enhancing the performance of redox flow batteries Here we propose a computational procedure for a systematic evaluation of organic redox-active species by combining machine learning, quantum-mechanical, and classical density functional theory calculations. 1,517 small quinone molecules were generated from the building blocks of benzoquinone, naphthoquinone, and anthraquinone with different substituent groups. The physics-based methods were used to predict HOMO-LUMO gaps and solvation free energies that account for the redox potential differences and aqueous solubility, respectively. The high-throughput calculations were augmented with the quantitative structure-property relationship analyses and machine learning/graph network modeling to evaluate the materials’ overall behavior. The computational procedure was able to reproduce high-performance cathode electrolyte materials consistent with experimental observations and identify new electrolytes for RFBs by screening 100,000 di-substituted quinone molecules, the largest library of redox-active quinone molecules ever investigated. The efficient computational platform may facilitate a better understanding of the structure-function relationship of quinone molecules and advance the design and application of all-organic active materials for RFBs.
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来源期刊
CiteScore
3.50
自引率
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