Heuristics for Molten-Salt Synthesis of Single-Crystalline Ultrahigh-Nickel Layered Oxide Cathodes

Mesnier, Alex; Manthiram, Arumugam

doi:10.1021/acsami.2c16326

Heuristics for Molten-Salt Synthesis of Single-Crystalline Ultrahigh-Nickel Layered Oxide Cathodes

Journal Article · Wed Mar 01 00:00:00 EST 2023 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.2c16326· OSTI ID:1972452

Mesnier, Alex ^[1]; ^[2]

Univ. of Texas at Austin, TX (United States); University of Texas at Austin
Univ. of Texas at Austin, TX (United States)

In pursuit of Li-ion batteries with higher energy density, ultrahigh-nickel layered oxides are a leading candidate for next-generation cathode materials. Single-crystalline morphology offers a neat solution to the poor stability of ultrahigh-Ni cathodes; a lower active surface area mitigates electrolyte decomposition at high voltages, and the elimination of grain boundaries improves mechanical resilience and increases volumetric energy density. However, single-crystal cathodes possess their own challenges, several of which originate from synthesis at elevated temperatures meant to induce grain growth. Molten-salt synthesis is an alternative method for obtaining single crystals, accelerating grain growth through the presence of a molten flux without the need for increased temperature. Herein, we offer heuristic guidelines for molten-salt synthesis, discussing key factors for designing reaction mixtures and the necessary exploratory research for novel molten salt/cathode systems. Here, the influence of different salts and synthesis conditions on the morphology and properties of single-crystal LiNiO₂ is presented. It is found that oxidative salts, such as Li₂O₂ and LiNO₃, are crucial to supplementing dissolution of gaseous oxygen into the molten phase. Through these discussions, this work aims to provide a set of overarching principles for obtaining higher-quality single-crystal layered oxide cathodes and engender more rigorous and impactful investigation into their fundamental nature and applications.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Texas at Austin, TX (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO)

Grant/Contract Number:: EE0008445

OSTI ID:: 1972452

Alternate ID(s):: OSTI ID: 2326349

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 10 Vol. 15; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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