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

Title data

Ma, Yanjiao ; Ma, Yuan ; Dreyer, Sören Lukas ; Wang, Qingsong ; Wang, Kai ; Goonetilleke, Damian ; Omar, Ahmad ; Mikhailova, Daria ; Hahn, Horst ; Breitung, Ben ; Brezesinski, Torsten:
High-Entropy Metal–Organic Frameworks for Highly Reversible Sodium Storage.
In: Advanced Materials. Vol. 33 (2021) Issue 34 . - No. 2101342.
ISSN 1521-4095

Official URL: Volltext

Project information

Project title:
Project's official title
Project's id
Nachwuchsgruppe Lehrstuhl für Anorganische Aktivmaterialien electrochemischer Speicher Dr. Qingsong Wang
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Abstract in another language

Abstract 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.

Further data

Item Type: Article in a journal
Refereed: Yes
Keywords: gassing behavior; high-entropy materials; Prussian blue analogues; secondary batteries; sodium-ion cathodes
Institutions of the University: Faculties > Faculty of Biology, Chemistry and Earth Sciences > Department of Chemistry
Faculties > Faculty of Biology, Chemistry and Earth Sciences > Department of Chemistry > Lehrstuhl Anorganische Aktivmaterialien für elektrochemische Energiespeicher
Research Institutions > Research Centres > Bayerisches Zentrum für Batterietechnik - BayBatt
Faculties > Faculty of Biology, Chemistry and Earth Sciences
Research Institutions
Research Institutions > Research Centres
Result of work at the UBT: No
DDC Subjects: 500 Science > 500 Natural sciences
500 Science > 540 Chemistry
600 Technology, medicine, applied sciences > 620 Engineering
Date Deposited: 02 Nov 2022 09:37
Last Modified: 02 Nov 2022 09:37