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High‐Entropy Metal–Organic Frameworks for Highly Reversible Sodium Storage

Ma, Yanjiao ; Ma, Yuan ; Dreyer, Sören Lukas ; Wang, Qingsong ; Wang, Kai ; Goonetilleke, Damian ; Omar, Ahmad ; Mikhailova, Daria ; Hahn, Horst ; Breitung, Ben ; Brezesinski, Torsten (2024)
High‐Entropy Metal–Organic Frameworks for Highly Reversible Sodium Storage.
In: Advanced Materials, 2021, 33 (34)
doi: 10.26083/tuprints-00021010
Article, Secondary publication, Publisher's Version

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Item Type: Article
Type of entry: Secondary publication
Title: High‐Entropy Metal–Organic Frameworks for Highly Reversible Sodium Storage
Language: English
Date: 22 January 2024
Place of Publication: Darmstadt
Year of primary publication: 2021
Place of primary publication: Weinheim
Publisher: Wiley-VCH
Journal or Publication Title: Advanced Materials
Volume of the journal: 33
Issue Number: 34
Collation: 10 Seiten
DOI: 10.26083/tuprints-00021010
Corresponding Links:
Origin: Secondary publication DeepGreen

Prussian blue analogues (PBAs) are reported to be efficient sodium storage materials because of the unique advantages of their metal–organic framework structure. However, the issues of low specific capacity and poor reversibility, caused by phase transitions during charge/discharge cycling, have thus far limited the applicability of these materials. Herein, a new approach is presented to substantially improve the electrochemical properties of PBAs by introducing high entropy into the crystal structure. To achieve this, five different metal species are introduced, sharing the same nitrogen‐coordinated site, thereby increasing the configurational entropy of the system beyond 1.5R. By careful selection of the elements, high‐entropy PBA (HE‐PBA) presents a quasi‐zero‐strain reaction mechanism, resulting in increased cycling stability and rate capability. The key to such improvement lies in the high entropy and associated effects as well as the presence of several active redox centers. The gassing behavior of PBAs is also reported. Evolution of dimeric cyanogen due to oxidation of the cyanide ligands is detected, which can be attributed to the structural degradation of HE‐PBA during battery operation. By optimizing the electrochemical window, a Coulombic efficiency of nearly 100% is retained after cycling for more than 3000 cycles.

Uncontrolled Keywords: gassing behavior, high‐entropy materials, Prussian blue analogues, secondary batteries, sodium‐ion cathodes
Identification Number: 2101342
Status: Publisher's Version
URN: urn:nbn:de:tuda-tuprints-210102
Classification DDC: 600 Technology, medicine, applied sciences > 660 Chemical engineering
Divisions: 11 Department of Materials and Earth Sciences > Material Science > Joint Research Laboratory Nanomaterials
Date Deposited: 22 Jan 2024 13:36
Last Modified: 16 Feb 2024 12:50
SWORD Depositor: Deep Green
URI: https://tuprints.ulb.tu-darmstadt.de/id/eprint/21010
PPN: 515590126
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