Chimie Douce Derived Novel P2‐Type Layered Oxide for Potassium‐Ion Batteries

Author:

Jha Pawan Kumar1,Golubnichiy Alexander2,Sachdeva Dorothy3,Banerjee Abhik4,Sai Gautam Gopalakrishnan5,Fichtner Maximilian67,Abakumov Artem M.2,Barpanda Prabeer167ORCID

Affiliation:

1. Faraday Materials Laboratory (FaMaL) Materials Research Center Indian Institute of Science Bangalore 560012 India

2. Center for Energy Science and Technology Skolkovo Institute of Science and Technology Bolshoi blv. 30–1 Moscow 121205 Russia

3. Materials Research Centre Indian Institute of Science Bangalore 560012 India

4. Research Institute for Sustainable Energy (RISE) TCG Centres for Research and Education in Science and Technology Sector V, Salt Lake Kolkata 700091 India

5. Department of Materials Engineering Indian Institute of Science Bangalore 560012 India

6. Helmholtz Institute Ulm (HIU) Electrochemical Energy Storage 89081 Ulm Germany

7. Institute of Nanotechnology Karlsruhe Institute of Technology (KIT) 76021 Karlsruhe Germany

Abstract

AbstractThe emergence of K‐ion batteries (KIBs) heralds a promising frontier in energy storage technology, offering the potential for high specific energy density, long cycle life, and robust power capabilities, all while utilizing the abundant resources of potassium. In response to the challenges posed by synthetic intricacies related to K‐based cathodes, the effort is directed toward employing soft chemistry (chimie douce) method to unveil a hitherto‐unknown P2‐type K1/3Co1/3Mn2/3O2 (KCM) layered oxide cathode for KIBs. Comprehensive analysis using diffraction, microscopy, and spectroscopy tools reveals the ion exchange reaction proceeds through overlay ordered structure formation mechanism. The as‐prepared KCM material serves as a ≈2.9 V positive K+ insertion host. Further, it showcases an exceptional structural reversibility, robust cycling performance with ≈100% coulombic efficiency even after 100 cycles, and maintaining electrochemical stability even at elevated temperature (c.a. 40° and 50 °C). The KCM cathode exhibits in‐plane Co–Mn ordering and solid‐solution redox mechanism during (de)potassiation. Combining first‐principles calculations with experimental tools, this research demonstrates the efficacy of ambient ion‐exchange route in stabilizing promising cathode materials for KIBs. This innovative synthetic approach not only streamlines synthetic complexities, but also holds significant implications for the advancement of KIB technology for stationary energy storage.

Funder

Science and Engineering Research Board

Russian Science Foundation

Alexander von Humboldt-Stiftung

Mission on Nano Science and Technology

Ministry of Education, India

Publisher

Wiley

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