Role of Cations in the Cation-Driven Assembly Process and their Effect on the Charge Storage Properties of Bilayered Vanadium Oxide and Reduced Graphene Oxide Heterostructures in Alkali Ion Systems

Andris, Ryan; Omo-Lamai, Darrell; Zachman, Michael J.; Pomerantseva, Ekaterina

doi:10.1021/acsaem.3c01440

Role of Cations in the Cation-Driven Assembly Process and their Effect on the Charge Storage Properties of Bilayered Vanadium Oxide and Reduced Graphene Oxide Heterostructures in Alkali Ion Systems

Journal Article · Mon Sep 18 00:00:00 EDT 2023 · ACS Applied Energy Materials

DOI:https://doi.org/10.1021/acsaem.3c01440· OSTI ID:2573529

^[1]; Omo-Lamai, Darrell ^[1]; ^[2]; ^[1]

Drexel Univ., Philadelphia, PA (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

Exfoliated δ-Li_xV₂O₅·nH₂O (ex-LVO) and reduced graphene oxide (rGO) heterostructures were constructed using different assembling cations (i.e., Li⁺, Na⁺, and K⁺ ions). The ex-LVO and rGO nanoflakes were stacked together using a concentrated chloride solution of each assembling cation and vacuum annealed at 200 °C to form three distinct two-dimensional (2D) layered architectures. X-ray diffraction and thermogravimetric analysis confirmed that the assembling ions can control the interlayer spacing of the bilayered vanadium oxide (BVO) phase as well as impact the crystallographic water content, which in turn affects the electrochemical performance. Scanning electron microscopy, scanning transmission electron microscopy (STEM), electron energy-loss spectroscopy (EELS), and X-ray photoelectron spectroscopy confirmed that a 2D heterointerface formed between LVO and rGO and that the cations used to assemble the heterostructure are trapped in the interlayer BVO region. High-resolution STEM imaging also showed the rGO dispersion throughout the LVO layers. Moreover, STEM-EELS identified a V₂O₃ phase that forms along the rGO interface and can stabilize the materials during cycling. A charge storage mechanism analysis, combined with the galvanostatic intermittent titration technique, found that increased interlayer spacings of the BVO phase and using the assembling cations to define intercalation sites for identical charge-carrying ions lead to improved ion diffusion and increased capacities during cycling. Therefore, the Li⁺ and Na⁺ ion assembled heterostructures showed improved charge-carrying ion diffusion and charge storage capacities in each of their respective charge storage systems (i.e., Li-ion and Na-ion half-cells). In total, the cation used for heterostructure assembly can modify the final material structure and tailor the ion diffusion and charge storage capacity to tune its properties for the desired electrochemical system using a variety of 2D materials.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 2573529

Journal Information:: ACS Applied Energy Materials, Journal Name: ACS Applied Energy Materials Journal Issue: 19 Vol. 6; ISSN 2574-0962

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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