Lean‐Water Hydrogel with Multipolar Sites for Flexible and High‐Performance Aqueous Aluminum Ion Batteries

Lean‐Water Hydrogel with Multipolar Sites for Flexible and High‐Performance Aqueous Aluminum Ion Batteries

Advanced Materials

10.1002/adma.202500695

https://doi.org/10.1002/adma.202500695

Ziyue Wen, Feng Wu, Man‐Fai Ng, Beier Jia, Jinxuan Song, Tianyang Yu, Jinfeng Dong, Anchun Tang, Renjie Chen, Qingyu Yan

General Materials Science

04 March 2025

Wen, Z., Wu, F., Ng, M.-F., Jia, B., Song, J., Yu, T., Dong, J., Tang, A., Chen, R., & Yan, Q. (2025). Lean‐Water Hydrogel with Multipolar Sites for Flexible and High‐Performance Aqueous Aluminum Ion Batteries. Advanced Materials, 37(15). Portico. https://doi.org/10.1002/adma.202500695

Rechargeable aqueous aluminum ion batteries (AAIBs) offer a promising avenue for achieving safe, high-energy and low-cost large-scale energy storage applications. However, the practical development of AAIBs is hindered by competitive reduction reactions in the aqueous solution, which lead to insufficient aluminum (Al) deposition and a severe hydrogen evolution reaction (HRE). In this work, an inorganic/organic hybrid hydrogel with a stable silicon-based network and multiple polar sites was successfully fabricated via an in-situ sol-gel polymerization method. The preferential formation of hydrogen bonds between the polar functional groups (-C=O and -NH) and water molecules effectively reduces the thermodynamic reactivity of water. Furthermore, X-ray photoelectron spectroscopy (XPS) and time of flight secondary ion mass spectrometry (TOF-SIMS) analyses confirm the formation of a stable, inorganic rich solid electrolyte interface (SEI) layer, which kinetically suppresses undesirable side reactions. This hydrogel electrolyte exhibits a high ionic conductivity of 2.9×10-3 S cm-1 at 25 ℃, even under lean-water conditions. As a result, Al|hydrogel|KNHCF full cells demonstrate excellent cycling performance, delivering a high initial discharge capacity of 74.9 mAh g-1 at 100 mA g-1 and achieving an outstanding capacity retention of 90.0 % after 200 cycles. Additionally, pouch cells exhibit stable open-circuit voltage under various mechanical abuse conditions. This work provides a promising approach for designing hydrogel electrolytes to enable high-performance and flexible AAIBs.

Publisher Copyright

This research / project is supported by the A*STAR - Manufacturing, Trade, and Connectivity Programmatic Fund - Physics and Knowledge Transfer-base d Cognitive Digital Twin for Advanced Battery Analytics
Grant Reference no. : M23L9B0052

This is the peer reviewed version of the following article: Wen, Z., Wu, F., Ng, M.-F., Jia, B., Song, J., Yu, T., Dong, J., Tang, A., Chen, R., & Yan, Q. (2025). Lean‐Water Hydrogel with Multipolar Sites for Flexible and High‐Performance Aqueous Aluminum Ion Batteries. Advanced Materials, 37(15). Portico. https://doi.org/10.1002/adma.202500695 , which has been published in final form at https://doi.org/10.1002/adma.202500695. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions. This article may not be enhanced, enriched or otherwise transformed into a derivative work, without express permission from Wiley or by statutory rights under applicable legislation. Copyright notices must not be removed, obscured or modified. The article must be linked to Wiley’s version of record on Wiley Online Library and any embedding, framing or otherwise making available the article or pages thereof by third parties from platforms, services and websites other than Wiley Online Library must be prohibited.

https://oar.a-star.edu.sg/communities-collections/articles/23265

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