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Applications of Ceramic/Graphene Composites and Hybrids materials Review Applications of Ceramic/Graphene Composites and Hybrids Cristina Ramírez *, Manuel Belmonte , Pilar Miranzo and Maria Isabel Osendi * Instituto de Cerámica y Vidrio (ICV), Consejo Superior de Investigaciones Científicas, CSIC. Kelsen 5, 28049 Madrid, Spain; [email protected] (M.B.); [email protected] (P.M.) * Correspondence: [email protected] (C.R.); [email protected] (M.I.O.); Tel.: +34-917-355-840 (C.R.); +34-917-355-868 (M.I.O.) Abstract: Research activity on ceramic/graphene composites and hybrids has increased dramatically in the last decade. In this review, we provide an overview of recent contributions involving ceramics, graphene, and graphene-related materials (GRM, i.e., graphene oxide, reduced graphene oxide, and graphene nanoplatelets) with a primary focus on applications. We have adopted a broad scope of the term ceramics, therefore including some applications of GRM with certain metal oxides and cement- based matrices in the review. Applications of ceramic/graphene hybrids and composites cover many different areas, in particular, energy production and storage (batteries, supercapacitors, solar and fuel cells), energy harvesting, sensors and biosensors, electromagnetic interference shielding, biomaterials, thermal management (heat dissipation and heat conduction functions), engineering components, catalysts, etc. A section on ceramic/GRM composites processed by additive manufacturing methods is included due to their industrial potential and waste reduction capability. All these applications of ceramic/graphene composites and hybrids are listed and mentioned in the present review, ending with the authors’ outlook of those that seem most promising, based on the research efforts carried out in this field. Keywords: ceramic graphene composites; ceramic graphene hybrids; applications; ceramic compos- Citation: Ramírez, C.; Belmonte, M.; Miranzo, P.; Osendi, M.I. ites; graphene; graphene-related materials; graphene oxide; graphene nanoplatelets Applications of Ceramic/Graphene Composites and Hybrids. Materials 2021, 14, 2071. https://doi.org/ 10.3390/ma14082071 1. Introduction Since the monolayer isolation in 2004, graphene has been a field of incessant activity, Academic Editor: Lei Zhai owing to the amazing properties of graphene [1] and the scope of potential applications and uses, as stated in many articles and reviews [2,3]. Focusing on the field of ceramic/graphene Received: 25 March 2021 composites and hybrids, the bustle relatively dims down, nevertheless, there has been Accepted: 16 April 2021 permanent growth in the number of published papers since 2004 as can be seen in Figure1a Published: 20 April 2021 (data collected from the Web of Science (WOS) with the topic graphene + ceramic + com- posite). Several reviews reflect the interest in this topic, revealing the benefits of graphene Publisher’s Note: MDPI stays neutral and related materials (GRM)-graphene oxide (GO), reduced graphene oxide (rGO), and with regard to jurisdictional claims in graphene nanoplatelets (GNP) as reinforcing agents that provide electrical and thermal published maps and institutional affil- transport properties or wear and friction benefits as well [3,4]. The increase in the number iations. of documents published since 2017 is particularly noticeable, so this review aims to offer a representative description of the most relevant contributions during the 2016–2020 five- year period but concentrating on applications, which have resulted in about 340 references from a total of almost 1000 papers in the period. The applications of ceramic/graphene Copyright: © 2021 by the authors. composites and hybrids include materials for energy production and storage, sensors, Licensee MDPI, Basel, Switzerland. tissue engineering, electromagnetic interference shields, thermal management, thermal This article is an open access article protection, protection against wear and corrosion, and uses in catalysis, each of which is distributed under the terms and discussed in the appropriate section, listed as follows: conditions of the Creative Commons Attribution (CC BY) license (https:// 2. Ceramic/graphene composites used in energy production and storage creativecommons.org/licenses/by/ 3. Piezo and thermoelectric ceramic/graphene composites for energy harvesting 4.0/). 4. Sensors based on ceramic/graphene composites and hybrids Materials 2021, 14, 2071. https://doi.org/10.3390/ma14082071 https://www.mdpi.com/journal/materials Materials 2021, 14, x FOR PEER REVIEW 2 of 64 4. Sensors based on ceramic/graphene composites and hybrids 5. Ceramic/graphene composites for electromagnetic interference shielding 6. Catalytic applications of ceramic/graphene composites 7. Ceramic/graphene composites in biomedicine 8. Thermal applications of ceramic/graphene composites 9. Structural engineering applications of ceramic/graphene composites 10. Applications of additively-manufactured ceramic/graphene composites In some cases, we have taken an ample view including inorganic materials such as metal oxides and cements, and in most cases, a slight account of the material fabrication procedure is included along with key results for the intended uses. Outcomes about composite materials fabricated by additive manufacturing methods that emphasize ap- plications deserved a separate section because they offer interesting flexibility and po- tential for novel device development. The number of patents filed in the subject (ceramic +graphene +composites) has ex- perienced an evolution quite similar to that of research articles (Figure 1b) but obviously with fewer documents. Despite these impressive figures, commercial product develop- Materials 2021, 14, 2071 ment clearly falls behind, and one of the alleged reasons is the relatively high cost2 of of 62 GRM, with figures on the order of 1250–2500 €/kg for GO, and much lower (100–700 €/kg) for GNP [5,6], both being the most widely used products in composite fabrication. On the positive side, it is important to notice that small amounts of these GRM (typically < 10 vol.%)5. Ceramic/graphene make a true impact composites on the properties for electromagnetic of composite interference materials shieldingowing to their pre- 6. Catalytic applications of ceramic/graphene composites sumably high exfoliation. The main impediments for mass industrialization are linked to 7. Ceramic/graphene composites in biomedicine reliability and quality control of GRM, although some authors point the finger at the ab- 8. Thermal applications of ceramic/graphene composites sence of a really groundbreaking application for graphene as [6]. However, favorable 9. Structural engineering applications of ceramic/graphene composites prospects lie ahead regarding production cost and quality control assessments for gra- 10. Applications of additively-manufactured ceramic/graphene composites phene materials and composites [5]. Figure 1. (a) PublicationsPublications per yearyear inin thethe subjectsubject ofof ceramic/grapheneceramic/graphene composites (data collected from WOS, Clarivate Analytics); ( b)) Number of of patents per year and cumulative in in the sa sameme topic in either the title or the abstract (source Espacenet, EPO). 2. Ceramic/GrapheneIn some cases, we Composites have taken Used an ample in Energy view includingProduction inorganic and Storage materials such as metal oxides and cements, and in most cases, a slight account of the material fabrication 2.1. Batteries procedure is included along with key results for the intended uses. Outcomes about com- positeThe materials increasing fabricated demand by additivefor portable manufacturing electronic methods devices that and emphasize electric vehicles applications has generateddeserved aenormous separate section research because efforts they to improv offer interestinge specific capacity, flexibility energy and potential density, for cycling novel performancedevice development. and safety of batteries used in energy storage systems. One of the recent strategiesThe numberto address of patentsthese challenges filed in the involves subject incorporating (ceramic + graphene GRM into + composites)battery compo- has nentsexperienced for improved an evolution electrochemical quite similar performance to that of research due to articles graphene´s (Figure excellent1b) but obviously electrical andwith thermal fewer documents. conductivities, Despite lightweight, these impressive high figures,specific commercialsurface area product and superior development me- chanicalclearly falls strength behind, [7]. andThe oneprincipal of the effects alleged of reasons adding is GRM the relativelyare: (i) improvement high cost of of GRM, the activewith figures material on distribution, the order of (ii) 1250–2500 control of€ /kgvolumetric for GO, expansion and much during lower cycling, (100–700 and€/kg) (iii) for GNP [5,6], both being the most widely used products in composite fabrication. On the positive side, it is important to notice that small amounts of these GRM (typically < 10 vol.%) make a true impact on the properties of composite materials owing to their presumably high exfoliation. The main impediments for mass industrialization are linked to reliability and quality control of GRM, although some authors point the finger at the absence of a really groundbreaking application for graphene as [6]. However, favorable prospects lie ahead regarding production cost and quality control assessments for graphene materials and composites [5]. 2. Ceramic/Graphene Composites Used in Energy Production
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