High‐energy‐density storage devices play a major role in modern electronics from traditional lithium‐ion batteries to supercapacitors for a variety of applications from rechargeable devices to advanced military equipment. Despite the mass adoption of polymer capacitors, their application is limited by their low energy densities and low‐temperature tolerance. Polymer nanocomposites based on 2D nanomaterials have superior capacitive energy densities, higher thermal stabilities, and higher mechanical strength as compared to the pristine polymers and nanocomposites based on 0D or 1D nanomaterials, thus making them ideal for high‐energy‐density dielectric energy storage applications. Here, the recent advances in 2D‐nanomaterial‐based nanocomposites and their implications for energy storage applications are reviewed. Nanocomposites based on conducting 2D nanofillers such as graphene, reduced graphene oxide, MXenes, semiconducting 2D nanofillers including transition metal dichalcogenides such as MoS2, dielectric 2D nanofillers including hBN, Mica, Al2O3, TiO2, Ca2Nb3O10and MMT, and their effects on permittivity, dielectric strength, capacitive energy density, efficiency, thermal stability, and the mechanical strength, are discussed. Also, the theory and machine‐learning‐guided design of polymer 2D nanomaterial composites is learnt and the challenges and opportunities for developing ultrahigh‐capacitive‐energy‐density devices based on these nanofiller polymer composites are presented.
more »
« less
This content will become publicly available on July 5, 2026
Transition Metal Modification of Graphene Oxide Membranes for Enhanced Aqueous Stability and Dielectric Performance
Graphene oxide (GO) membranes, known for their high dielectric constant and low dielectric loss, have emerged as promising separators for advanced energy storage and transfer devices. While previous research has focused on the aqueous stability enhancement by high-valence metal cations, their effect on modifying the dielectric properties of GO membranes remains understudied. This study investigates the impact of transition metal cation modification on the aqueous stability and dielectric properties of graphene oxide (GO) membranes. Multivalent transition metal chlorides (FeCl3, FeCl2, CuCl2, and CuCl) were introduced during the self-assembly process to create modified GO membranes. The membranes were characterized using various techniques, including zeta potential measurements, contact angle measurements, FTIR spectroscopy, and XRD spectroscopy. The aqueous stability of the modified membranes was evaluated, and their dielectric performance was assessed using capacitance measurements across a frequency range of 0.1 Hz to 105 Hz. The results demonstrate that the choice of transition metal cation and its oxidation state significantly influence the morphology, aqueous stability, and dielectric properties of the GO membranes. Notably, Fe3+ and Cu2+ modifications enhanced aqueous stability, while Fe2+ and Cu+ modifications improved dielectric performance. This study provides insights into tailoring the properties of GO membranes for various applications, including energy storage and transfer devices.
more »
« less
- Award ID(s):
- 2301838
- PAR ID:
- 10579637
- Publisher / Repository:
- Elsevier
- Date Published:
- Journal Name:
- Colloids and Surfaces A: Physicochemical and Engineering Aspects
- Volume:
- 716
- ISSN:
- 0927-7757
- Page Range / eLocation ID:
- 136737
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Graphene and graphene oxide have shown good antibacterial activity against different bacterial species due to their unique physicochemical properties. Graphene oxide (GO) has been widely used to load metallic and metal oxide nanoparticles (NPs) to minimize their surface energy during processing and preparation, hence reducing their aggregation. In this work, GO was effectively synthesized and coated with different concentrations of zinc hydroxide Zn (OH)x using the precipitation method to prepare a GO/Zn (OH)x hybrid composite. The Zn (OH)x NPs and GO/Zn (OH)x nanocomposites were synthesized and characterized using various methods such as scanning electron microscopy (SEM), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). Coating GO with Zn (OH)x NPs resulted in improved aggregation of Zn (OH)x NPs as well as enhanced antibacterial activity of GO against Gram-positive and Gram-negative bacteria. Additionally, the effect of Zn (OH)x coating on the antibacterial properties of the GO/Zn (OH)x composite was systematically investigated. The synergistic effects of GO and Zn (OH)x NPs resulted in enhanced antibacterial properties of the composites compared to the pristine GO material. In addition, increasing the Zn (OH)x wt. % concentration led to an increased inhibition zone of the GO/Zn (H)x composite against Bacillus megaterium and E. coli bacteria.more » « less
-
Graphene oxide (GO) films have a great potential for aerospace, electronics, and renewable energy applications due to their low cost and unique properties. For structural applications, they can achieve an exceptional combination of damping and stiffness. This study investigates the effect of packing density, reduction, and water removal on stiffness and damping of graphene oxide films. GO sheets dispersed in water are passed through a filter and deposited on a removable substrate. Through variations of the film fabrication process, films of both GO and reduced GO (rGO) are produced with varying levels of packing. Heat treatment is also used to remove the water in half of the films. The degree of packing is assessed through film density calculations. Microscopy as well as Raman and X-ray spectroscopy are used to measure the degree of packing while Dynamic Mechanical Analysis (DMA) is used to quantity mechanical damping and storage modulus of specimens in tension. Correlating mechanical properties to structure of films revealed new understanding of damping and stress transfer mechanisms in these materials. Optimal structures resulted in superior combinations of stiffness (18 GPa) and damping (0.14), potentially paving the way for using GO based films in advanced structural applications.more » « less
-
Recently, graphene fibers derived from wet-spinning of graphene oxide (GO) dispersions have emerged as viable electrodes for fiber-shaped supercapacitors (FSCs) and/or batteries, wherein large surface area, high electrical conductivity, and sufficient mechanical strength/toughness are desired. However, for most fiber electrodes reported so far, compromises have to be made between energy-storage capacity and mechanical/electrical performance, whereas a graphene fiber with high capacity and sufficient toughness for direct machine weaving or knitting is yet to be developed. Inspired by the alum mordant used for natural dyes in the traditional textile dyeing industry, our research group has synthesized wet-spun GO fibers and coagulated them with different multivalent cations ( e.g. Ca 2+ , Fe 3+ , and Al 3+ ), where dramatically different fiber morphologies and properties have been observed. The first principles density functional theory has been further employed to explain the observed disparities via cation–GO binding energy calculation. When assembled into solid-state FSCs, Al 3+ -based reduced GO (rGO) fibers offer excellent stability against bending, and a specific capacitance of 148.5 mF cm −2 at 40 mV s −1 , 1.4, 4.8, and 6.8 times higher than that of the rGO fibers based on other three coagulation systems (Fe 3+ , Ca 2+ and acetic acid), respectively. The volumetric energy density of the Al 3+ -based FSC is up to 13.26 mW h cm −3 , while a high power density of 250.87 mW cm −3 is maintained.more » « less
-
Layer-stacked graphene oxide (GO) membranes, in which unique two-dimensional (2D) water channels are formed between two neighboring GO nanosheets, have demonstrated great potential for aqueous phase separation. Subjects of crucial importance are to fundamentally understand the interlayer spacing ( i.e. channel height) of GO membranes in an aqueous environment, elucidate the mechanisms for water transport within such 2D channels, and precisely control the interlayer spacing to tune the membrane separation capability for targeted applications. In this investigation, we used an integrated quartz crystal mass balance (QCM-D) and ellipsometry to experimentally monitor the interlayer spacing of GO, reduced GO and crosslinked GO in aqueous solution and found that crosslinking can effectively prevent GO from swelling and precisely control the interlayer spacing. We then used molecular dynamics simulations to study the mass transport inside the 2D channels and proved that the chemical functional groups on the GO plane dramatically slow down water transport in the channels. Our findings on GO structure and water transport provide a necessary basis for further tailoring and optimizing the design and fabrication of GO membranes in various separation applications.more » « less
An official website of the United States government
