3f8f76743127457615b92d7044796fac pmc_35159858.pdf ef6041b0436ef33006b98c2e303975c1c0bc5b70 pmc_35159858.pdf f6bfa262ea10f79c12bfd6f11368d4f477b31ec232b7c1f46c562f0f623e5427 pmc_35159858.pdf Title: Coherent Integration of Organic Gel Polymer Electrolyte and Ambipolar Polyoxometalate Hybrid Nanocomposite Electrode in a Compact High-Performance Supercapacitor Subject: We report a gel polymer electrolyte (GPE) supercapacitor concept with improved pathways for ion transport, thanks to a facile creation of a coherent continuous distribution of the electrolyte throughout the electrode. Poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) was chosen as the polymer framework for organic electrolytes. A permeating distribution of the GPE into the electrodes, acting both as integrated electrolyte and binder, as well as thin separator, promotes ion diffusion and increases the active electrode–electrolyte interface, which leads to improvements both in capacitance and rate capability. An activation process induced during the first charge–discharge cycles was detected, after which, the charge transfer resistance and Warburg impedance decrease. We found that a GPE thickness of 12 m led to optimal capacitance and rate capability. A novel hybrid nanocomposite material, formed by the tetraethylammonium salt of the 1 nm-sized phosphomolybdate cluster and activated carbon (AC/TEAPMo12), was shown to improve its capacitive performance with this gel electrolyte arrangement. Due to the homogeneous dispersion of PMo12 clusters, its energy storage process is non-diffusion-controlled. In the symmetric capacitors, the hybrid nanocomposite material can perform redox reactions in both the positive and the negative electrodes in an ambipolar mode. The volumetric capacitance of a symmetric supercapacitor made with the hybrid electrodes increased by 40% compared to a cell with parent AC electrodes. Due to the synergy between permeating GPE and the hybrid electrodes, the GPE hybrid symmetric capacitor delivers three times more energy density at higher power densities and equivalent cycle stability compared with conventional AC symmetric capacitors. Keywords: gel polymer electrolytes; polyoxometalates; supercapacitors; hybrid electrodes; organic electrolytes; impedance spectroscopy Author: Jun-Jie Zhu, Luis Martinez-Soria and Pedro Gomez-Romero Creator: LaTeX with hyperref Producer: pdfTeX-1.40.21 CreationDate: Wed Feb 9 09:28:09 2022 CET ModDate: Wed Feb 9 10:21:34 2022 CET Tagged: no UserProperties: no Suspects: no Form: none JavaScript: no Pages: 14 Encrypted: no Page size: 595.276 x 841.89 pts (A4) Page rot: 0 File size: 3797558 bytes Optimized: no PDF version: 1.7 name type encoding emb sub uni object ID ------------------------------------ ----------------- ---------------- --- --- --- --------- OVNEXW+EURM10 Type 1 Builtin yes yes no 10 0 KKVSGU+URWPalladioL-Bold Type 1 Custom yes yes no 14 0 EBKYTJ+URWPalladioL-Roma Type 1 Custom yes yes no 19 0 INJUEW+URWPalladioL-Ital Type 1 Custom yes yes no 23 0 PSUYZB+VnURWPalladioL Type 1 Custom yes yes no 27 0 MCBCCI+SourceSansRoman-Regular Type 1C Custom yes yes no 36 0 MCBCCM+SourceSansRoman.613wght Type 1C Custom yes yes no 40 0 MCBCCO+SourceSansRoman-Bold Type 1C Custom yes yes no 44 0 NPLVPL+TimesNewRomanPS-BoldItalicMT Type 1C WinAnsi yes yes no 56 0 UCWJLP+CMSY10 Type 1 Builtin yes yes no 81 0 SPXLNH+PazoMath Type 1 Builtin yes yes no 94 0 TSEGZF+PazoMath-Bold Type 1 Builtin yes yes no 101 0 RFLZJB+CMR10 Type 1 Builtin yes yes no 126 0 Jhove (Rel. 1.22.1, 2019-04-17) Date: 2022-04-01 02:22:32 CEST RepresentationInformation: pmc_35159858.pdf ReportingModule: PDF-hul, Rel. 1.12.1 (2019-04-17) LastModified: 2022-02-27 18:43:50 CET Size: 3797558 Format: PDF Version: 1.7 Status: Well-Formed and valid SignatureMatches: PDF-hul MIMEtype: application/pdf PDFMetadata: Objects: 279 FreeObjects: 1 IncrementalUpdates: 0 DocumentCatalog: PageLayout: SinglePage PageMode: UseNone Outlines: Item: Title: Introduction Destination: edu.harvard.hul.ois.jhove.module.pdf.PdfSimpleObject@7b69c6ba Item: Title: Experimental Section Destination: edu.harvard.hul.ois.jhove.module.pdf.PdfSimpleObject@46daef40 Children: Item: Title: Materials Destination: edu.harvard.hul.ois.jhove.module.pdf.PdfSimpleObject@12f41634 Item: Title: Preparation of Gel Electrolytes Destination: edu.harvard.hul.ois.jhove.module.pdf.PdfSimpleObject@13c27452 Item: Title: Synthesis of Hybrid Materials Destination: edu.harvard.hul.ois.jhove.module.pdf.PdfSimpleObject@262b2c86 Item: Title: Preparation of Electrodes Destination: edu.harvard.hul.ois.jhove.module.pdf.PdfSimpleObject@371a67ec Item: Title: Characterization Destination: edu.harvard.hul.ois.jhove.module.pdf.PdfSimpleObject@5ed828d Item: Title: Results and Discussion Destination: edu.harvard.hul.ois.jhove.module.pdf.PdfSimpleObject@50d0686 Children: Item: Title: Evaluation and Optimization of GPE Destination: edu.harvard.hul.ois.jhove.module.pdf.PdfSimpleObject@7a3d45bd Item: Title: Evaluation of the Hybrid Material Destination: edu.harvard.hul.ois.jhove.module.pdf.PdfSimpleObject@1e7c7811 Item: Title: Evaluation of Symmetric Devices Destination: edu.harvard.hul.ois.jhove.module.pdf.PdfSimpleObject@77ec78b9 Item: Title: Conclusions Destination: edu.harvard.hul.ois.jhove.module.pdf.PdfSimpleObject@1a3869f4 Item: Title: References Destination: edu.harvard.hul.ois.jhove.module.pdf.PdfSimpleObject@a38d7a3 Info: Title: Coherent Integration of Organic Gel Polymer Electrolyte and Ambipolar Polyoxometalate Hybrid Nanocomposite Electrode in a Compact High-Performance Supercapacitor Author: Jun-Jie Zhu, Luis Martinez-Soria and Pedro Gomez-Romero Subject: We report a gel polymer electrolyte (GPE) supercapacitor concept with improved pathways for ion transport, thanks to a facile creation of a coherent continuous distribution of the electrolyte throughout the electrode. Poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) was chosen as the polymer framework for organic electrolytes. A permeating distribution of the GPE into the electrodes, acting both as integrated electrolyte and binder, as well as thin separator, promotes ion diffusion and increases the active electrode electrolyte interface, which leads to improvements both in capacitance and rate capability. An activation process induced during the first charge discharge cycles was detected, after which, the charge transfer resistance and Warburg impedance decrease. We found that a GPE thickness of 12 m led to optimal capacitance and rate capability. A novel hybrid nanocomposite material, formed by the tetraethylammonium salt of the 1 nm-sized phosphomolybdate cluster and activated carbon (AC/TEAPMo12), was shown to improve its capacitive performance with this gel electrolyte arrangement. Due to the homogeneous dispersion of PMo12 clusters, its energy storage process is non-diffusion-controlled. In the symmetric capacitors, the hybrid nanocomposite material can perform redox reactions in both the positive and the negative electrodes in an ambipolar mode. The volumetric capacitance of a symmetric supercapacitor made with the hybrid electrodes increased by 40% compared to a cell with parent AC electrodes. Due to the synergy between permeating GPE and the hybrid electrodes, the GPE hybrid symmetric capacitor delivers three times more energy density at higher power densities and equivalent cycle stability compared with conventional AC symmetric capacitors. 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