2026-01-13 アルゴンヌ国立研究所（ANL）
＜関連情報＞
- https://www.anl.gov/article/autonomous-discoverydriven-argonne-study-inspires-paradigm-shift-in-battery-research
- https://pubs.acs.org/doi/10.1021/jacs.5c10140
ハイスループット発見により、有機電解質中の長寿命荷電種の設計原理と限界が明らかに High-Throughput Discovery Illuminates Design Principles and Limits for Long-Lived Charged Species in Organic Electrolytes
Lily A. Robertson,Ilya A. Shkrob,Ryan Lewis,Logan Ward,Rafael Vescovi,and Benjamin T. Diroll
Journal of American Chemical Society Published September 18, 2025
DOI:https://doi.org/10.1021/jacs.5c10140
Abstract
The chemical stability of charged molecules in all-organic redox flow batteries (RFBs) is required for the prolonged operation of these devices. Molecular engineering and electrolyte optimization are used to mitigate parasitic reactions and extend the lifetimes of the charge carriers. However, how much can structural variation extend the lifetime? To probe this query, we designed a high-throughput kinetic study of the radical cation of N-methylphenothiazinium, guided by statistical sampling and learning algorithms. Using Argonne’s autonomous discovery facility, we conducted over 6,000 kinetic experiments with robotic sample preparation, parallel kinetic measurements, and machine learning inputs, testing 188 solvent molecules selected from a space of over 540 candidates from 11 chemical classes. Algorithmic selections guided us to stable solvent candidates, which were further tested in high concentration with and without supporting electrolyte. Our findings reveal the inherent difficulty of exceeding the current state of the art through solvent variation. The desired stability is statistically rare and poorly predictable. Among the many tested, only three solvents significantly outperformed our baseline, acetonitrile─and none by more than a factor of 3─suggesting a general challenge in achieving the necessary techno-economic targets. We suggest that self-discharge through solvent homolysis is the cause of the observed limitations. Several structural motifs contribute to >1,000 h half-life stability including molecular simplicity, symmetry, oxidation complement, and strategic fluorination. Importantly, this workflow establishes effective assays for diagnosing and predicting oxidative stress for highly stable liquid electrolytes in all batteries.
