Macromolecular Design Strategies for Preventing Active-Material Crossover in Non-Aqueous All-Organic Redox-Flow Batteries

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• 作者：Sean E. Doris ; Dr. Ashleigh L. Ward ; Dr. Artem Baskin ; Dr. Peter D. Frischmann ; Dr. Nagarjuna Gavvalapalli ; Dr. Etienne Ché ; nard ; Dr. Christo S. Sevov ; Dr. David Prendergast ; Prof. Jeffrey S. Moore and Dr. Brett A. Helms
• 刊名：Angewandte Chemie International Edition
• 出版年：2017
• 出版时间：February 1, 2017
• 年：2017
• 卷：56
• 期：6
• 页码：1595-1599
• 全文大小：2227K
• ISSN：1521-3773

文摘

Intermittent energy sources, including solar and wind, require scalable, low-cost, multi-hour energy storage solutions in order to be effectively incorporated into the grid. All-Organic non-aqueous redox-flow batteries offer a solution, but suffer from rapid capacity fade and low Coulombic efficiency due to the high permeability of redox-active species across the battery's membrane. Here we show that active-species crossover is arrested by scaling the membrane's pore size to molecular dimensions and in turn increasing the size of the active material above the membrane's pore-size exclusion limit. When oligomeric redox-active organics (RAOs) were paired with microporous polymer membranes, the rate of active-material crossover was reduced more than 9000-fold compared to traditional separators at minimal cost to ionic conductivity. This corresponds to an absolute rate of RAO crossover of less than 3 μmol cm⁻² day⁻¹ (for a 1.0 m concentration gradient), which exceeds performance targets recently set forth by the battery industry. This strategy was generalizable to both high and low-potential RAOs in a variety of non-aqueous electrolytes, highlighting the versatility of macromolecular design in implementing next-generation redox-flow batteries.