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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.
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Capacitive Enhancement Mechanisms and Design Principles of High‐Performance Graphene Oxide‐Based All‐Solid‐State Supercapacitors
Abstract Graphene oxide (GO)‐based all‐solid‐state supercapacitors (GO‐A3Ss) are superior over liquid electrolyte‐based supercapacitors and capable of being integrated on a single chip in various geometry shapes for the use of future smart wearable electronics field as a fast energy storage device, but their capacitance need to be improved. Here, a new approach has been developed for enhancing the capacitive capability of the supercapacitors through molecular dynamics simulations with the first‐principle input. A theoretical model of charge storage is developed to understand the unique capacitive enhancement mechanism and to predict the capacitance of the GO‐A3Ss, which agrees well with the experimental observations. A novel supercapacitor with GO and reduced graphene oxide (rGO) alternatively layered structures is designed based on the model, and its energy density is the highest among conventional supercapacitors using liquid electrolytes and all‐solid‐state supercapacitors using aerogels or hydrogels as the solid‐state electrolyte. Based on the predictions, two new types of high‐performance GO/rGO multilayered capacitors are proposed to meet different practical applications. The results of this work provide an approach for the design of high‐performance all‐solid‐state supercapacitors based on GO and rGO materials.
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- Award ID(s):
- 1662288
- PAR ID:
- 10053656
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Functional Materials
- Volume:
- 28
- Issue:
- 17
- ISSN:
- 1616-301X
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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