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- Transport and Energy Processes at Electrochemical Interfaces I
- (111c) Pressurized Organic Electrodes Enable Practical/Extreme Batteries
2025 AIChE Annual Meeting
(111c) Pressurized Organic Electrodes Enable Practical/Extreme Batteries
Author
Organic batteries hold promise for sustainable development due to their natural abundance, tunable structures, low emissions, and potential cost-effectiveness. Over recent decades, numerous organics (comprising C, O, N, and S moieties) have been explored as battery electrode materials, spanning lithium, sodium, and zinc-ion batteries. Strategies have emerged to enhance battery performance via molecular design, polymer engineering, carbon hybridization, micro-/nanostructure construction, and electrolyte/separator modification. However, their practical applications still face grand challenges due to impractical testing conditions and elevated costs.
Organic materials of limited conductivity typically necessitate substantial quantities of conductive carbon, resulting in a lower fraction of active materials (AM, 30-70 wt.%) in electrodes, notably less than the 90-97 wt.% achieved with commercial inorganic counterparts. Composed of light elements, organic materials inherently possess low density, and the density of resulting electrodes is even lower (e.g., 0.2 g cm-3) due to design of porous structure and presence of considerable carbon. This combined low density and AM fraction is usually accompanied with low mass loadings (typically 1-2 mg cm-2) in organic electrodes, compromising cell-level energy densities. Ongoing efforts have sought to address these issues, yet yielding limited success. Moreover, most reported organic batteries are tested in half-cell or three-electrode configuration, lacking control over the N/P ratio and electrolyte quantity, while some organic syntheses involve complex and costly catalyst-dependent processes. Overall, practical organic batteries must excel under the “three high three low (3H3L)” condition: high mass loading, AM fraction, and density, while maintaining cost-effectiveness, low N/P ratios, and minimized electrolyte in full-cell setups. Unfortunately, very few endeavors have simultaneously met demanding "3H3L" criteria. Solutions to break the current bottleneck remain an open challenge.
Organic materials of limited conductivity typically necessitate substantial quantities of conductive carbon, resulting in a lower fraction of active materials (AM, 30-70 wt.%) in electrodes, notably less than the 90-97 wt.% achieved with commercial inorganic counterparts. Composed of light elements, organic materials inherently possess low density, and the density of resulting electrodes is even lower (e.g., 0.2 g cm-3) due to design of porous structure and presence of considerable carbon. This combined low density and AM fraction is usually accompanied with low mass loadings (typically 1-2 mg cm-2) in organic electrodes, compromising cell-level energy densities. Ongoing efforts have sought to address these issues, yet yielding limited success. Moreover, most reported organic batteries are tested in half-cell or three-electrode configuration, lacking control over the N/P ratio and electrolyte quantity, while some organic syntheses involve complex and costly catalyst-dependent processes. Overall, practical organic batteries must excel under the “three high three low (3H3L)” condition: high mass loading, AM fraction, and density, while maintaining cost-effectiveness, low N/P ratios, and minimized electrolyte in full-cell setups. Unfortunately, very few endeavors have simultaneously met demanding "3H3L" criteria. Solutions to break the current bottleneck remain an open challenge.
Inspired by pressure-enabled structural and performance modification in superconductors, optoelectronics, and cell stacks, we report the making of pressurized organic electrodes (POE) for practical batteries under “3H3L” condition. The pressure effects on the structure, property, and performance of organic materials/electrodes were systematically investigated. Under high pressure, a series of changes occur: morphological transformation, enhanced π-π interaction, narrowed band gap, vacancy formation, crystal orientation, porosity/tortuosity change as well as increased density, chemical reactivity, electronic conductivity, thermal stability, mechanical strength, and adhesive property. As a result, organic electrodes treated with higher pressure demonstrate better capacity, rate, and cycling performance in batteries. Under harsh condition of high-loading electrodes (51 mg cm-2), low N/P ratio (0.84), lean electrolyte (2.1 μL mg-1), a POE-based full cell demonstrates high areal capacity (6.6 mAh cm-2), fast charging capability (12 min) and a thousand cycle life with high initial Coulombic efficiency (CE) of 94.5% and stable CE of >99.95%. POE also enables extreme batteries working under ultrahigh mass loadings of 150 mg cm-2 (capacity: 22.5 mAh) and AM fraction of 95% (energy density: 112.6 Wh L-1), far surpassing previous organic batteries. Moreover, POE technology could be broadly applied to different battery systems and organic materials, demonstrating one of highest areal capacities (3-18 mAh cm-2) with leanest electrolyte among all reports. This establishes POE as a simple yet powerful technology for the practical implementation of organic electrodes.