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

Ma, Yanjiao 1; Ma, Yuan 1; Dreyer, Sören Lukas 1; Wang, Qingsong 1; Wang, Kai 1; Goonetilleke, Damian 1; Omar, Ahmad; Mikhailova, Daria; Hahn, Horst 1; Breitung, Ben ORCID iD icon 1; Brezesinski, Torsten ORCID iD icon 1
1 Institut für Nanotechnologie (INT), Karlsruher Institut für Technologie (KIT)


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. ... mehr

Verlagsausgabe §
DOI: 10.5445/IR/1000136003
Veröffentlicht am 30.07.2021
DOI: 10.1002/adma.202101342
Zitationen: 142
Web of Science
Zitationen: 135
Zitationen: 150
Cover der Publikation
Zugehörige Institution(en) am KIT Institut für Nanotechnologie (INT)
Publikationstyp Zeitschriftenaufsatz
Publikationsdatum 26.08.2021
Sprache Englisch
Identifikator ISSN: 0935-9648, 1521-4095
KITopen-ID: 1000136003
HGF-Programm 43.31.02 (POF IV, LK 01) Devices and Applications
Weitere HGF-Programme 38.02.01 (POF IV, LK 01) Fundamentals and Materials
Erschienen in Advanced Materials
Verlag John Wiley and Sons
Band 33
Heft 34
Seiten Art. Nr.: 2101342
Vorab online veröffentlicht am 09.07.2021
Nachgewiesen in Scopus
Web of Science
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