Entropy‐Regulated Cathode with Low Strain and Constraint Phase‐Change Toward Ultralong‐Life Aqueous Al‐Ion Batteries

Author:

Liu Yan‐Ning1,Yang Jia‐Lin2,Gu Zhen‐Yi2,Zhang Xin‐Yi1,Liu Yue2,Su Meng‐Yuan1,Zhang Xue‐Li1,Zatovsky Igor V.3,Li Kai4,Cao Jun‐Ming2ORCID,Wu Xing‐Long12ORCID

Affiliation:

1. Department of Chemistry Northeast Normal University Changchun Jilin 130024 P. R. China

2. MOE Key Laboratory for UV Light-Emitting Materials and Technology Northeast Normal University Changchun Jilin 130024 P. R. China

3. F.D. Ovcharenko Institute of Biocolloidal Chemistry NAS Ukraine, 42 Acad. Vernadskoho blv. 03142 Kyiv Ukraine

4. State Key Laboratory of Rare Earth Resource Utilization Institute of Applied Chemistry Chinese Academy of Sciences Changchun 130022 P. R. China

Abstract

AbstractDuring multivalent ions insertion processes, intense electrostatic interaction between charge carriers and host makes the high‐performance reversible Al3+ storage remains an elusive target. On account of the strong electrostatic repulsion and poor robustness, Prussian Blue analogues (PBAs) suffer severely from the inevitable and large strain and phase change during reversible Al3+ insertion. Herein, we demonstrate an entropy‐driven strategy to realize ultralong life aqueous Al‐ion batteries (AIBs) based on medium entropy PBAs (ME‐PBAs) host. By multiple redox active centers introduction, the intrinsic poor conductivity can be enhanced simultaneously, resulting in outstanding capabilities of electrochemical Al3+ storage. Meanwhile, the co‐occupation at metal sites in PBA frameworks can also increase the M−N bond intensity, which is beneficial for constraining the phase change during consecutive Al3+ reversible insertion, to realize an extended lifespan over 10,000 cycles. Based on the calculation at different operation states, the fluctuation of ME‐PBA lattice parameters is only 1.2 %. Assembled with MoO3 anodes, the full cells can also deliver outstanding electrochemical properties. The findings highlight that, the entropy regulation strategy could uncover the isochronous constraint on both strain and phase transition for long‐term reversible Al3+ storage, providing a promising design for advanced electrode materials for aqueous multivalent ions batteries.

Funder

National Key Research and Development Program of China

National Natural Science Foundation of China

Publisher

Wiley

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