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

© 2021 The Authors. Advanced Materials published by Wiley-VCH GmbH.

Bibliographische Detailangaben
Veröffentlicht in:Advanced materials (Deerfield Beach, Fla.). - 1998. - 33(2021), 34 vom: 24. Aug., Seite e2101342
1. Verfasser: Ma, Yanjiao (VerfasserIn)
Weitere Verfasser: Ma, Yuan, Dreyer, Sören Lukas, Wang, Qingsong, Wang, Kai, Goonetilleke, Damian, Omar, Ahmad, Mikhailova, Daria, Hahn, Horst, Breitung, Ben, Brezesinski, Torsten
Format: Online-Aufsatz
Sprache:English
Veröffentlicht: 2021
Zugriff auf das übergeordnete Werk:Advanced materials (Deerfield Beach, Fla.)
Schlagworte:Journal Article Prussian blue analogues gassing behavior high-entropy materials secondary batteries sodium-ion cathodes
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520 |a 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 
650 4 |a Journal Article 
650 4 |a Prussian blue analogues 
650 4 |a gassing behavior 
650 4 |a high-entropy materials 
650 4 |a secondary batteries 
650 4 |a sodium-ion cathodes 
700 1 |a Ma, Yuan  |e verfasserin  |4 aut 
700 1 |a Dreyer, Sören Lukas  |e verfasserin  |4 aut 
700 1 |a Wang, Qingsong  |e verfasserin  |4 aut 
700 1 |a Wang, Kai  |e verfasserin  |4 aut 
700 1 |a Goonetilleke, Damian  |e verfasserin  |4 aut 
700 1 |a Omar, Ahmad  |e verfasserin  |4 aut 
700 1 |a Mikhailova, Daria  |e verfasserin  |4 aut 
700 1 |a Hahn, Horst  |e verfasserin  |4 aut 
700 1 |a Breitung, Ben  |e verfasserin  |4 aut 
700 1 |a Brezesinski, Torsten  |e verfasserin  |4 aut 
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773 1 8 |g volume:33  |g year:2021  |g number:34  |g day:24  |g month:08  |g pages:e2101342 
856 4 0 |u http://dx.doi.org/10.1002/adma.202101342  |3 Volltext 
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