Entropy‐Mediated Stable Structural Evolution of Prussian White Cathodes for Long‐Life Na‐Ion Batteries

Author:

He Yueyue1,Dreyer Sören L.1,Ting Yin‐Ying23,Ma Yuan1,Hu Yang4,Goonetilleke Damian15,Tang Yushu1,Diemant Thomas4,Zhou Bei1,Kowalski Piotr M.36,Fichtner Maximilian4,Hahn Horst17,Aghassi‐Hagmann Jasmin1,Brezesinski Torsten1ORCID,Breitung Ben1ORCID,Ma Yanjiao18ORCID

Affiliation:

1. Institute of Nanotechnology Karlsruhe Institute of Technology (KIT) Hermann-von-Helmholtz Platz 1 76344 Eggenstein-Leopoldshafen Germany

2. Institute of Energy and Climate Research (IEK-13) Forschungszentrum Jülich GmbH Wilhelm-Johnen-Str. 52428 Jülich Germany

3. Chair of Theory and Computation of Energy Materials Faculty of Georesources and Materials Engineering RWTH Aachen University 52062 Aachen Germany

4. Helmholtz Institute Ulm (HIU) for Electrochemical Energy Storage Helmholtzstr. 11 89081 Ulm Germany

5. Current address: Corporate Research and Development, Umicore Watertorenstraat 33 2250 Olen Belgium

6. Jülich Aachen Research Alliance JARA Energy & Center for Simulation and Data Science (CSD) 52425 Jülich Germany

7. School of Chemical Biological and Materials Engineering The University of Oklahoma Norman OK, 73019 USA

8. Current address: School of Energy and Mechanical Engineering Jiangsu Key Laboratory of New Power Batteries Nanjing Normal University Nanjing 210023 China

Abstract

AbstractThe high‐entropy approach is applied to monoclinic Prussian White (PW) Na‐ion cathodes to address the issue of unfavorable multilevel phase transitions upon electrochemical cycling, leading to poor stability and capacity decay. A series of Mn‐based samples with up to six metal species sharing the N‐coordinated positions was synthesized. The material of composition Na1.65Mn0.4Fe0.12Ni0.12Cu0.12Co0.12Cd0.12[Fe(CN)6]0.920.08 ⋅ 1.09H2O was found to exhibit superior cyclability over medium/low‐entropy and conventional single‐metal PWs. We also report, to our knowledge for the first time, that a high‐symmetry crystal structure may be advantageous for high‐entropy PWs during battery operation. Computational comparisons of the formation enthalpy demonstrate that the compositionally less complex materials are prone to phase transitions, which negatively affect cycling performance. Based on data from complementary characterization techniques, an intrinsic mechanism for the stability improvement of the disordered PW structure upon Na+ insertion/extraction is proposed, namely the dual effect of suppression of phase transitions and mitigation of gas evolution.

Funder

Chinese Government Scholarship

Deutsche Forschungsgemeinschaft

Publisher

Wiley

Subject

General Medicine

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