Search NASA⌕ Search
Home/Archive/DOE OSTI

DOE OSTI · 3451495

Electrostatic‐Attraction‐Driven Self‐Assembled Graphene‐Disordered Rocksalt Composite Cathode for Lithium‐Ion Batteries

Avvaru, Venkata Sai [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)]·Zuba, Mateusz [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000232097922)·Armstrong, Beth L. [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)] (ORCID:0000000171493576)·Wang, Shilong [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States)]·Tran, Minh X. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)]·Rinkel, Bernardine L. D. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States)]·Babbe, Finn [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)]·Lohani, Harshita [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)]·Fu, Yanbao [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)]·Buyuker, Isik Su [Argonne National Laboratory (ANL), Argonne, IL (United States)]·Battaglia, Vincent [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)]·Kahvecioglu, Ozgenur [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000239883301)·Kostecki, Robert [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)]·McCloskey, Bryan D. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States)]·Kim, Haegyeom [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)]
View original source ↗Read source document ↗Export metadata ↓

Abstract

Disordered rocksalt cathodes hold promise for achieving high-capacity lithium-ion batteries while using low-cost, earth-abundant elements. However, their electrochemical performance remains critically limited by their poor electronic conductivity. Conventional strategies such as high-energy ball milling with excess carbon additives can improve conductivity but remain challenging to scale and often produce defects and increase surface area, thereby accelerating capacity degradation. Herein, we report an alternative approach of electrostatic-attraction-driven self-assembly to fabricate Li 1.2 Mn 0.6 Ti 0.2 O 1.8 F 0.2 (LMTOF) particles uniformly wrapped with electronically conductive graphene sheets without associated materials degradation. The graphene-wrapped LMTOF demonstrates significantly improved cycling stability (89% capacity retention after 100 cycles) and superior rate capability compared with an LMTOF-carbon composite electrode fabricated using the conventional high-energy ball-milling process. Post-cycling analysis reveals reduced oxygen evolution, suppressed unwanted side reactions, and improved structural integrity for the graphene-LMTOF composite. This work highlights the advantages of solution-based carbon wrapping and offers a scalable strategy to prepare high-performance DRX cathodes for lithium-ion batteries.

Explore related subjects

carbon compositecathodesdisordered rocksaltgraphenelithium-ion batteriessolution-based synthesis

Keep this discovery

BibTeXRIS

Avvaru, Venkata Sai [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)], Zuba, Mateusz [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000232097922), Armstrong, Beth L. [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)] (ORCID:0000000171493576), Wang, Shilong [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States)], Tran, Minh X. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)], Rinkel, Bernardine L. D. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States)], Babbe, Finn [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)], Lohani, Harshita [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)], Fu, Yanbao [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)], Buyuker, Isik Su [Argonne National Laboratory (ANL), Argonne, IL (United States)], Battaglia, Vincent [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)], Kahvecioglu, Ozgenur [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000239883301), Kostecki, Robert [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)], McCloskey, Bryan D. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States)], Kim, Haegyeom [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)]. 2026-07-10. Electrostatic‐Attraction‐Driven Self‐Assembled Graphene‐Disordered Rocksalt Composite Cathode for Lithium‐Ion Batteries. https://doi.org/10.1002/adfm.76964

Cite the original work for its findings. Save a collection to share your selection of sources.

Discover connections

Carbon composites materialLithium-ion batteries materialLithium-ion batteries subjectcarbon composite subjectcathodes subjectdisordered rocksalt subjectgraphene subject

Connections use source metadata and explicit phrase matches, not verified experimental comparisons.

KEEP EXPLORING

Related discoveries

DOE OSTI2025

Modeling phase transformations in Mn-rich disordered rocksalt cathodes with machine-learning interatomic potentials

Mn-rich disordered rocksalt (DRX) cathode materials exhibit a phase transformation from a disordered to a partially disordered spinel-like structure (δ-phase) during electrochemical cycling. Here, in this computational study, we use charge-informed molecular dynamics with a fine-tuned CHGNet foundation potential to investigate the phase transformation in LixMn 0.8 Ti 0.1 O 1.9 F 0.1 . Our results indicate that transition metal migration occurs and reorders to form the spinel-like ordering in an FCC anion framework. The transformed structure contains a higher concentration of nontransition metal (0-TM) face-sharing channels, which are known to improve Li transport kinetics. Analysis of the Mn valence distribution suggests that the appearance of tetrahedral Mn 2+ is a consequence of spinel-like ordering, rather than the trigger for cation migration as previously suggested. Calculated equilibrium intercalation voltage profiles demonstrate that the δ-phase, unlike the ordered spinel, exhibits solid-solution signatures at low voltage. A higher Li capacity is obtained than in the DRX phase. This study provides atomic insights into solid-state phase transformation and its relation to experimental electrochemistry, highlighting the potential of machine-learning interatomic potentials for understanding complex oxide materials.

Zhong, Peichen [University of California, Berkeley↗
DOE OSTI2026

Visualizing Crystallization Dynamics and Transformation Pathways of Disordered Rocksalt Oxides During Thermally Activated Sol–Gel Synthesis

Sol–gel synthesis is a wet-chemical processing route for fabricating functional materials with control over composition and microstructure at relatively low temperatures compared to conventional solid-state synthesis. While sol–gel process initiates with intermixed molecular precursors, the early-stage nucleation pathways are insufficiently understood. Here, in this study, the chemical and structural transformation of ion disordered rocksalt (DRX) Li 1.2 Mn 0.4 Ti 0.4 O 2 (LMTO), a promising cathode material for lithium batteries, is studied by multiscale characterizations. In situ heating transmission electron microscopy (TEM) using a liquid cell visualizes and identifies crystallization pathways at the nanoscale. While some regions follow a classical multi-step transition through thermodynamically stable intermediates, others exhibit a kinetic shortcut via a localized amorphous matrix to directly form the DRX structure. Macroscale Fourier transform infrared spectroscopy corroborates the findings and reveals that transition metal ions are more strongly incorporated into the acetate-coordinated network than lithium. Although in situ heating TEM captures diverse local transformation pathways, in situ synchrotron X-ray diffraction indicates that the macroscopic transformation proceeds predominantly through spinel LMTO and lithium titanates toward DRX-LMTO. The findings uncover the spatiotemporal chemical and structural transformations in sol–gel derived DRX-LMTO materials, and call for fine-tuning of such sol–gel chemistries to manipulate the crystallization pathways and achieve target material homogeneity more efficiently.

cathode material↗