Abstract

Lithium preintercalated bilayered vanadium oxide (LVO or δ-Li_xV₂O₅·nH₂O) and graphene oxide (GO) nanoflakes were assembled using a concentrated lithium chloride solution and annealed under vacuum at 200 °C to form two-dimensional (2D) δ-Li_xV₂O₅·nH₂O and reduced GO (rGO) heterostructures. Here we found that the Li⁺ ions from LiCl enhanced the oxide/carbon heterointerface formation and served as stabilizing ions to improve structural and electrochemical stability. The graphitic content of the heterostructure could be easily controlled by changing the initial GO concentration prior to assembly. We found that increasing the GO content in our heterostructure composition helped inhibit the electrochemical degradation of LVO during cycling and improved the rate capability of the heterostructure. A combination of scanning electron microscopy and X-ray diffraction was used to help confirm that a 2D heterointerface formed between LVO and GO, and the final phase composition was determined using energy-dispersive X-ray spectroscopy and thermogravimetric analysis. Scanning transmission electron microscopy and electron energy-loss spectroscopy were additionally used to examine the heterostructures at high resolution, mapping the orientations of rGO and LVO layers and locally imaging their interlayer spacings. Further, electrochemical cycling of the cation-assembled LVO/rGO heterostructures in Li-ion cells with a non-aqueous electrolyte revealed that increasing the rGO contentmore » led to improved cycling stability and rate performance, despite slightly decreased charge storage capacity. The heterostructures with 0, 10, 20, and 35 wt % rGO exhibited capacities of 237, 216, 174, and 150 mAh g^–1, respectively. Moreover, the LVO/rGO-35 wt % and LVO/rGO-20 wt % heterostructures retained 75% (110 mAh g–1) and 67% (120 mAh g^–1) of their initial capacities after increasing the specific current from 20 to 200 mA g^–1, while the LVO/rGO-10 wt % sample retained only 48% (107 mAh g^–1) of its initial capacity under the same cycling conditions. In addition, the cation-assembled LVO/rGO electrodes exhibited enhanced electrochemical stability compared to electrodes prepared through physical mixing of LVO and GO nanoflakes in the same ratios as the heterostructure electrodes, further revealing the stabilizing effect of a 2D heterointerface. The cation-driven assembly approach, explored in this work using Li⁺ cations, was found to induce and stabilize the formation of stacked 2D layers of rGO and exfoliated LVO. The reported assembly methodology can be applied for a variety of systems utilizing 2D materials with complementary properties for applications as electrodes in energy storage devices.« less

Authors:

Andris, Ryan ^[1]; Averianov, Timofey ^[1]; Zachman, Michael J.  ^[2];

• Search DOE PAGES for author "Zachman, Michael J."
• Search DOE PAGES for ORCID "0000-0003-1910-1357"

Pomerantseva, Ekaterina  ^[1]

• Search DOE PAGES for author "Pomerantseva, Ekaterina"
• Search DOE PAGES for ORCID "0000-0002-6765-7133"

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+ Show Author Affiliations

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

Publication Date:

Mon May 22 00:00:00 EDT 2023

Research Org.:

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

Sponsoring Org.:

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

OSTI Identifier:

1999045

Grant/Contract Number:  

AC05-00OR22725; DMR-1752623

Resource Type:

Accepted Manuscript

Journal Name:

ACS Applied Materials and Interfaces

Additional Journal Information:

Journal Volume: 15; Journal Issue: 22; Journal ID: ISSN 1944-8244

Publisher:

American Chemical Society (ACS)

Country of Publication:

United States

Language:

English

Subject:

25 ENERGY STORAGE; bilayered vanadium oxide; reduced graphene oxide; liquid phase exfoliation; nanoflake assembly; 2D heterostructures; Li-on batteries