Special Issue "Graphene-Polymer Composites"

A special issue of Polymers (ISSN 2073-4360).

Deadline for manuscript submissions: closed (5 December 2017)

Printed Edition Available!
A printed edition of this Special Issue is available here.

Special Issue Editor

Guest Editor
Prof. Dr. Fernão D. Magalhães

LEPABE, Chemical Engineering Department, Faculty of Engineering, University of Porto, Portugal
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Interests: synthetic and natural adhesives, lignocellulosic composites, high-performance industrial coatings, graphene-based biomaterials

Special Issue Information

Dear Colleagues,

The mechanical, electrical, thermal, magnetic, optical and biological properties of graphene have attracted a significant amount of attention from the research community since the isolation of single-atom-thick graphene layers, by Geim and co-workers in 2004. Presenting very high surface-to-volume ratio, relatively simple processability and low cost, graphene and graphene-related materials were soon identified as promising nanofillers for polymer matrixes. Reports have shown notorious property enhancements for graphene-polymer composites (GPC) at very low filler loadings. Uses of GPC in varied fields, such as energy, electronics, catalysis, separation and purification, biomedicine, aerospace, tribology, etc., have been demonstrated and, in some cases, put into industrial practice. However, challenges still exist. Platelet agglomeration within the polymer matrix is often seen to hinder performance improvements. Poor interfacial adhesion between filler and matrix is also a limiting factor in many systems, demanding for tuning the surface chemistry to promote physical or chemical interactions with the polymer chains. The range of routes for fabrication of graphene-related materials, leading to different morphologies, oxidation states, and degrees of platelet exfoliation, have an impact on the final properties of the composites that has not yet been fully addressed. Some argue that the potential of graphene, and its advantages in relation to other nanofillers, has not yet been clearly demonstrated for polymer composites.

This Special Issue invites original papers and reviews reporting on recent progress in the following areas:

  • Chemical and physical surface modifications of graphene and graphene-related materials for improving dispersibility and compatibility with polymer matrixes.
  • Fabrication methods of GPC in coating, film, bulk or particulate forms.
  • Properties of GPC (chemical, mechanical, thermal, electrical, magnetic, etc.).
  • Biological and biomedical properties of GPC (biocompatibility, antimicrobial activity, etc.).
  • Applications of GPC.

It must be noted that the term “composite” should be understood here in its broader sense, describing a material, of any geometry and size, made of two or more constituent materials that do not lose their individual identities when combined.

Prof. Fernão D. Magalhães
Guest Editor

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Keywords

  • Graphene
  • Graphene oxide
  • Composites
  • Coatings
  • Adhesives
  • Fibers
  • Particles
  • Surface modification
  • Surface functionalization
  • Materials properties
  • Biological properties

Published Papers (12 papers)

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Research

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Open AccessArticle Effects of Carbon Nanotubes/Graphene Nanoplatelets Hybrid Systems on the Structure and Properties of Polyetherimide-Based Foams
Polymers 2018, 10(4), 348; https://doi.org/10.3390/polym10040348
Received: 31 January 2018 / Revised: 9 March 2018 / Accepted: 19 March 2018 / Published: 21 March 2018
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Abstract
Foams based on polyetherimide (PEI) with carbon nanotubes (CNT) and PEI with graphene nanoplatelets (GnP) combined with CNT were prepared by water vapor induced phase separation. Prior to foaming, variable amounts of only CNT (0.1–2.0 wt %) or a combination of GnP (0.0–2.0
[...] Read more.
Foams based on polyetherimide (PEI) with carbon nanotubes (CNT) and PEI with graphene nanoplatelets (GnP) combined with CNT were prepared by water vapor induced phase separation. Prior to foaming, variable amounts of only CNT (0.1–2.0 wt %) or a combination of GnP (0.0–2.0 wt %) and CNT (0.0–2.0 wt %) for a total amount of CNT-GnP of 2.0 wt %, were dispersed in a solvent using high power sonication, added to the PEI solution, and intensively mixed. While the addition of increasingly higher amounts of only CNT led to foams with more heterogeneous cellular structures, the incorporation of GnP resulted in foams with finer and more homogeneous cellular structures. GnP in combination with CNT effectively enhanced the thermal stability of foams by delaying thermal decomposition and mechanically-reinforced PEI. The addition of 1.0 wt % GnP in combination with 1.0 wt % CNT resulted in foams with extremely high electrical conductivity, which was related to the formation of an optimum conductive network by physical contact between GnP layers and CNT, enabling their use in electrostatic discharge (ESD) and electromagnetic interference (EMI) shielding applications. The experimental electrical conductivity values of foams containing only CNT fitted well to a percolative conduction model, with a percolation threshold of 0.06 vol % (0.1 wt %) CNT. Full article
(This article belongs to the Special Issue Graphene-Polymer Composites) Printed Edition available
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Open AccessArticle Permeability and Selectivity of PPO/Graphene Composites as Mixed Matrix Membranes for CO2 Capture and Gas Separation
Polymers 2018, 10(2), 129; https://doi.org/10.3390/polym10020129
Received: 5 December 2017 / Revised: 22 January 2018 / Accepted: 24 January 2018 / Published: 29 January 2018
Cited by 4 | PDF Full-text (18122 KB) | HTML Full-text | XML Full-text | Supplementary Files
Abstract
We fabricated novel composite (mixed matrix) membranes based on a permeable glassy polymer, Poly(2,6-dimethyl-1,4-phenylene oxide) (PPO), and variable loadings of few-layer graphene, to test their potential in gas separation and CO2 capture applications. The permeability, selectivity and diffusivity of different gases as
[...] Read more.
We fabricated novel composite (mixed matrix) membranes based on a permeable glassy polymer, Poly(2,6-dimethyl-1,4-phenylene oxide) (PPO), and variable loadings of few-layer graphene, to test their potential in gas separation and CO2 capture applications. The permeability, selectivity and diffusivity of different gases as a function of graphene loading, from 0.3 to 15 wt %, was measured at 35 and 65 °C. Samples with small loadings of graphene show a higher permeability and He/CO2 selectivity than pure PPO, due to a favorable effect of the nanofillers on the polymer morphology. Higher amounts of graphene lower the permeability of the polymer, due to the prevailing effect of increased tortuosity of the gas molecules in the membrane. Graphene also allows dramatically reducing the increase of permeability with temperature, acting as a “stabilizer” for the polymer matrix. Such effect reduces the temperature-induced loss of size-selectivity for He/N2 and CO2/N2, and enhances the temperature-induced increase of selectivity for He/CO2. The study confirms that, as observed in the case of other graphene-based mixed matrix glassy membranes, the optimal concentration of graphene in the polymer is below 1 wt %. Below such threshold, the morphology of the nanoscopic filler added in solution affects positively the glassy chains packing, enhancing permeability and selectivity, and improving the selectivity of the membrane at increasing temperatures. These results suggest that small additions of graphene to polymers can enhance their permselectivity and stabilize their properties. Full article
(This article belongs to the Special Issue Graphene-Polymer Composites) Printed Edition available
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Open AccessArticle Thermomechanical Behavior of Polymer Composites Based on Edge-Selectively Functionalized Graphene Nanosheets
Polymers 2018, 10(1), 29; https://doi.org/10.3390/polym10010029
Received: 21 November 2017 / Revised: 22 December 2017 / Accepted: 23 December 2017 / Published: 26 December 2017
Cited by 1 | PDF Full-text (6669 KB) | HTML Full-text | XML Full-text
Abstract
In this study, we demonstrate an effective approach based on a simple processing method to improve the thermomechanical properties of graphene polymer composites (GPCs). Edge-selectively functionalized graphene (EFG) was successfully obtained through simple ball milling of natural graphite in the presence of dry
[...] Read more.
In this study, we demonstrate an effective approach based on a simple processing method to improve the thermomechanical properties of graphene polymer composites (GPCs). Edge-selectively functionalized graphene (EFG) was successfully obtained through simple ball milling of natural graphite in the presence of dry ice, which acted as the source of carboxyl functional groups that were attached to the peripheral basal plane of graphene. The resultant EFG is highly dispersible in various organic solvents and contributes to improving their physical properties because of its unique characteristics. Pyromellitic dianhydride (PMDA) and 4,4′-oxydianiline (ODA) were used as monomers for constructing the polyimide (PI) backbone, after which PI/EFG composites were prepared by in situ polymerization. A stepwise thermal imidization method was used to prepare the PI films for comparison purposes. The PI/EFG composite films were found to exhibit reinforced thermal and thermo-mechanical properties compared to neat PI owing to the interaction between the EFG and PI matrix. Full article
(This article belongs to the Special Issue Graphene-Polymer Composites) Printed Edition available
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Open AccessArticle Improving Kinetics of “Click-Crosslinking” for Self-Healing Nanocomposites by Graphene-Supported Cu-Nanoparticles
Polymers 2018, 10(1), 17; https://doi.org/10.3390/polym10010017
Received: 5 December 2017 / Revised: 20 December 2017 / Accepted: 21 December 2017 / Published: 24 December 2017
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Abstract
Investigation of the curing kinetics of crosslinking reactions and the development of optimized catalyst systems is of importance for the preparation of self-healing nanocomposites, able to significantly extend their service lifetimes. Here we study different modified low molecular weight multivalent azides for a
[...] Read more.
Investigation of the curing kinetics of crosslinking reactions and the development of optimized catalyst systems is of importance for the preparation of self-healing nanocomposites, able to significantly extend their service lifetimes. Here we study different modified low molecular weight multivalent azides for a capsule-based self-healing approach, where self-healing is mediated by graphene-supported copper-nanoparticles, able to trigger “click”-based crosslinking of trivalent azides and alkynes. When monitoring the reaction kinetics of the curing reaction via reactive dynamic scanning calorimetry (DSC), it was found that the “click-crosslinking” reactivity decreased with increasing chain length of the according azide. Additionally, we could show a remarkable “click” reactivity already at 0 °C, highlighting the potential of click-based self-healing approaches. Furthermore, we varied the reaction temperature during the preparation of our tailor-made graphene-based copper(I) catalyst to further optimize its catalytic activity. With the most active catalyst prepared at 700 °C and the optimized set-up of reactants on hand, we prepared capsule-based self-healing epoxy nanocomposites. Full article
(This article belongs to the Special Issue Graphene-Polymer Composites) Printed Edition available
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Open AccessArticle Preparation of Electrospun Nanocomposite Nanofibers of Polyaniline/Poly(methyl methacrylate) with Amino-Functionalized Graphene
Polymers 2017, 9(9), 453; https://doi.org/10.3390/polym9090453
Received: 31 August 2017 / Revised: 11 September 2017 / Accepted: 12 September 2017 / Published: 16 September 2017
Cited by 2 | PDF Full-text (4667 KB) | HTML Full-text | XML Full-text
Abstract
In this paper we report upon the preparation and characterization of electrospun nanofibers of doped polyaniline (PANI)/poly(methyl methacrylate) (PMMA)/amino-functionalized graphene (Am-rGO) by electrospinning technique. The successful functionalization of rGO with amino groups is examined by Fourier transforms infrared (FTIR), X-ray photoelectron spectroscopy (XPS)
[...] Read more.
In this paper we report upon the preparation and characterization of electrospun nanofibers of doped polyaniline (PANI)/poly(methyl methacrylate) (PMMA)/amino-functionalized graphene (Am-rGO) by electrospinning technique. The successful functionalization of rGO with amino groups is examined by Fourier transforms infrared (FTIR), X-ray photoelectron spectroscopy (XPS) and Raman microspectrometer. The strong electric field enables the liquid jet to be ejected faster and also contributes to the improved thermal and morphological homogeneity of PANI/PMMA/Am-rGO. This results in a decrease in the average diameter of the produced fibers and shows that these fibers can find promising uses in many applications such as sensors, flexible electronics, etc. Full article
(This article belongs to the Special Issue Graphene-Polymer Composites) Printed Edition available
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Open AccessArticle Imidazolium Ionic Liquid Modified Graphene Oxide: As a Reinforcing Filler and Catalyst in Epoxy Resin
Polymers 2017, 9(9), 447; https://doi.org/10.3390/polym9090447
Received: 18 July 2017 / Revised: 28 August 2017 / Accepted: 11 September 2017 / Published: 14 September 2017
Cited by 5 | PDF Full-text (10566 KB) | HTML Full-text | XML Full-text
Abstract
Surface modification of graphene oxide (GO) is one of the most important issues to produce high performance GO/epoxy composites. In this paper, the imidazole ionic liquid (IMD-Si) was introduced onto the surface of GO sheets by a cheap and simple method, to prepare
[...] Read more.
Surface modification of graphene oxide (GO) is one of the most important issues to produce high performance GO/epoxy composites. In this paper, the imidazole ionic liquid (IMD-Si) was introduced onto the surface of GO sheets by a cheap and simple method, to prepare a reinforcing filler, as well as a catalyst in epoxy resin. The interlayer spacing of GO sheets was obviously increased by the intercalation of IMD-Si, which strongly facilitated the dispersibility of graphene oxide in organic solvents and epoxy matrix. The addition of 0.4 wt % imidazolium ionic liquid modified graphene oxide (IMD-Si@GO), yielded a 12% increase in flexural strength (141.3 MPa), a 26% increase in flexural modulus (4.69 GPa), and a 52% increase in impact strength (18.7 kJ/m2), compared to the neat epoxy. Additionally the IMD-Si@GO sheets could catalyze the curing reaction of epoxy resin-anhydride system significantly. Moreover, the improved thermal conductivities and thermal stabilities of epoxy composites filled with IMD-Si@GO were also demonstrated. Full article
(This article belongs to the Special Issue Graphene-Polymer Composites) Printed Edition available
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Open AccessArticle Effect of Graphene Oxide on the Reaction Kinetics of Methyl Methacrylate In Situ Radical Polymerization via the Bulk or Solution Technique
Polymers 2017, 9(9), 432; https://doi.org/10.3390/polym9090432
Received: 31 July 2017 / Revised: 27 August 2017 / Accepted: 5 September 2017 / Published: 8 September 2017
Cited by 2 | PDF Full-text (3666 KB) | HTML Full-text | XML Full-text
Abstract
The synthesis of nanocomposite materials based on poly(methyl methacrylate) and graphene oxide (GO) is presented using the in situ polymerization technique, starting from methyl methacrylate, graphite oxide, and an initiator, and carried out either with (solution) or without (bulk) in the presence of
[...] Read more.
The synthesis of nanocomposite materials based on poly(methyl methacrylate) and graphene oxide (GO) is presented using the in situ polymerization technique, starting from methyl methacrylate, graphite oxide, and an initiator, and carried out either with (solution) or without (bulk) in the presence of a suitable solvent. Reaction kinetics was followed gravimetrically and the appropriate characterization of the products took place using several experimental techniques. X-ray diffraction (XRD) data showed that graphite oxide had been transformed to graphene oxide during polymerization, whereas FTIR spectra revealed no significant interactions between the polymer matrix and GO. It appears that during polymerization, the initiator efficiency was reduced by the presence of GO, resulting in a reduction of the reaction rate and a slight increase in the average molecular weight of the polymer formed, measured by gel permeation chromatography (GPC), along with an increase in the glass transition temperature obtained from differential scanning calorimetry (DSC). The presence of the solvent results in the suppression of the gel-effect in the reaction rate curves, the synthesis of polymers with lower average molecular weights and polydispersities of the Molecular Weight Distribution, and lower glass transition temperatures. Finally, from thermogravimetric analysis (TG), it was verified that the presence of GO slightly enhances the thermal stability of the nano-hybrids formed. Full article
(This article belongs to the Special Issue Graphene-Polymer Composites) Printed Edition available
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Open AccessArticle Graphene Oxide-Graft-Poly(l-lactide)/Poly(l-lactide) Nanocomposites: Mechanical and Thermal Properties
Polymers 2017, 9(9), 429; https://doi.org/10.3390/polym9090429
Received: 31 July 2017 / Revised: 30 August 2017 / Accepted: 3 September 2017 / Published: 7 September 2017
Cited by 1 | PDF Full-text (2268 KB) | HTML Full-text | XML Full-text
Abstract
The surface modification of graphene sheets with polymer chains may greatly hinder its aggregation and improve its phase compatibility with a polymer matrix. In this work, poly(l-lactic acid)-grafted graphene oxide (GO-g-PLLA) was prepared via a simple condensation polymerization method, realizing its dispersion well
[...] Read more.
The surface modification of graphene sheets with polymer chains may greatly hinder its aggregation and improve its phase compatibility with a polymer matrix. In this work, poly(l-lactic acid)-grafted graphene oxide (GO-g-PLLA) was prepared via a simple condensation polymerization method, realizing its dispersion well in organic solvents, which demonstrated that the surface of GO changed from hydrophilic to hydrophobic. GO-g-PLLA can disperse homogeneously in the PLLA matrix, and the tensile test showed that the mechanical properties of GO-g-PLLA/PLLA were much better than that of GO/PLLA; compared with GO, only 3% GO-g-PLLA content can realize a 37.8% increase in the tensile strength for their PLLA composites. Furthermore, the differential scanning calorimetry (DSC) and polarized optical microscopy (POM) results demonstrated that GO-g-PLLA shows a nucleating agent effect and can promote the crystallization of PLLA. Full article
(This article belongs to the Special Issue Graphene-Polymer Composites) Printed Edition available
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Review

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Open AccessReview Recent Achievements of Self-Healing Graphene/Polymer Composites
Polymers 2018, 10(2), 114; https://doi.org/10.3390/polym10020114
Received: 21 December 2017 / Revised: 21 January 2018 / Accepted: 22 January 2018 / Published: 25 January 2018
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Abstract
Self-healing materials have attracted much attention because that they possess the ability to increase the lifetime of materials and reduce the total cost of systems during the process of long-term use; incorporation of functional material enlarges their applications. Graphene, as a promising additive,
[...] Read more.
Self-healing materials have attracted much attention because that they possess the ability to increase the lifetime of materials and reduce the total cost of systems during the process of long-term use; incorporation of functional material enlarges their applications. Graphene, as a promising additive, has received great attention due to its large specific surface area, ultrahigh conductivity, strong antioxidant characteristics, thermal stability, high thermal conductivity, and good mechanical properties. In this brief review, graphene-containing polymer composites with self-healing properties are summarized including their preparations, self-healing conditions, properties, and applications. In addition, future perspectives of graphene/polymer composites are briefly discussed. Full article
(This article belongs to the Special Issue Graphene-Polymer Composites) Printed Edition available
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Open AccessReview Intercalation Polymerization Approach for Preparing Graphene/Polymer Composites
Polymers 2018, 10(1), 61; https://doi.org/10.3390/polym10010061
Received: 5 December 2017 / Revised: 28 December 2017 / Accepted: 5 January 2018 / Published: 10 January 2018
Cited by 2 | PDF Full-text (15524 KB) | HTML Full-text | XML Full-text
Abstract
The rapid development of society has promoted increasing demand for various polymer materials. A large variety of efforts have been applied in order for graphene strengthened polymer composites to satisfy different requirements. Graphene/polymer composites synthesized by traditional strategies display some striking defects, like
[...] Read more.
The rapid development of society has promoted increasing demand for various polymer materials. A large variety of efforts have been applied in order for graphene strengthened polymer composites to satisfy different requirements. Graphene/polymer composites synthesized by traditional strategies display some striking defects, like weak interfacial interaction and agglomeration of graphene, leading to poor improvement in performance. Furthermore, the creation of pre-prepared graphene while being necessary always involves troublesome processes. Among the various preparation strategies, an appealing approach relies on intercalation and polymerization in the interlayer of graphite and has attracted researchers’ attention due to its reliable, fast and simple synthesis. In this review, we introduce an intercalation polymerization strategy to graphene/polymer composites by the intercalation of molecules/ions into graphite interlayers, as well as subsequent polymerization. The key point for regulating intercalation polymerization is tuning the structure of graphite and intercalants for better interaction. Potential applications of the resulting graphene/polymer composites, including electrical conductivity, electromagnetic absorption, mechanical properties and thermal conductivity, are also reviewed. Furthermore, the shortcomings, challenges and prospects of intercalation polymerization are discussed, which will be helpful to researchers working in related fields. Full article
(This article belongs to the Special Issue Graphene-Polymer Composites) Printed Edition available
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Open AccessReview Thermal Conductivity of Graphene-Polymer Composites: Mechanisms, Properties, and Applications
Polymers 2017, 9(9), 437; https://doi.org/10.3390/polym9090437
Received: 5 August 2017 / Revised: 7 September 2017 / Accepted: 7 September 2017 / Published: 15 September 2017
Cited by 19 | PDF Full-text (5667 KB) | HTML Full-text | XML Full-text
Abstract
With the integration and miniaturization of electronic devices, thermal management has become a crucial issue that strongly affects their performance, reliability, and lifetime. One of the current interests in polymer-based composites is thermal conductive composites that dissipate the thermal energy produced by electronic,
[...] Read more.
With the integration and miniaturization of electronic devices, thermal management has become a crucial issue that strongly affects their performance, reliability, and lifetime. One of the current interests in polymer-based composites is thermal conductive composites that dissipate the thermal energy produced by electronic, optoelectronic, and photonic devices and systems. Ultrahigh thermal conductivity makes graphene the most promising filler for thermal conductive composites. This article reviews the mechanisms of thermal conduction, the recent advances, and the influencing factors on graphene-polymer composites (GPC). In the end, we also discuss the applications of GPC in thermal engineering. This article summarizes the research on graphene-polymer thermal conductive composites in recent years and provides guidance on the preparation of composites with high thermal conductivity. Full article
(This article belongs to the Special Issue Graphene-Polymer Composites) Printed Edition available
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Open AccessReview Poly(lactic acid) Composites Containing Carbon-Based Nanomaterials: A Review
Polymers 2017, 9(7), 269; https://doi.org/10.3390/polym9070269
Received: 15 June 2017 / Revised: 30 June 2017 / Accepted: 4 July 2017 / Published: 6 July 2017
Cited by 13 | PDF Full-text (3283 KB) | HTML Full-text | XML Full-text
Abstract
Poly(lactic acid) (PLA) is a green alternative to petrochemical commodity plastics, used in packaging, agricultural products, disposable materials, textiles, and automotive composites. It is also approved by regulatory authorities for several biomedical applications. However, for some uses it is required that some of
[...] Read more.
Poly(lactic acid) (PLA) is a green alternative to petrochemical commodity plastics, used in packaging, agricultural products, disposable materials, textiles, and automotive composites. It is also approved by regulatory authorities for several biomedical applications. However, for some uses it is required that some of its properties be improved, namely in terms of thermo-mechanical and electrical performance. The incorporation of nanofillers is a common approach to attain this goal. The outstanding properties of carbon-based nanomaterials (CBN) have caused a surge in research works dealing with PLA/CBN composites. The available information is compiled and reviewed, focusing on PLA/CNT (carbon nanotubes) and PLA/GBM (graphene-based materials) composites. The production methods, and the effects of CBN loading on PLA properties, namely mechanical, thermal, electrical, and biological, are discussed. Full article
(This article belongs to the Special Issue Graphene-Polymer Composites) Printed Edition available
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