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Green Approaches to Carbon Nanostructure-Based Biomaterials

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Green Approaches to Carbon Nanostructure-Based Biomaterials applied sciences Review Green Approaches to Carbon Nanostructure-Based Biomaterials Simone Adorinni 1 , Maria C. Cringoli 1,2 , Siglinda Perathoner 3,4, Paolo Fornasiero 1,2,5 and Silvia Marchesan 1,2,* 1 Chemical and Pharmaceutical Sciences Department, University of Trieste, 34127 Trieste, Italy; [email protected] (S.A.); [email protected] (M.C.C.); [email protected] (P.F.) Review 2 INSTM, University of Trieste, 34127 Trieste, Italy Green Approaches3 Dipartimentoto Carbon di Scienze Na Chimiche,nostructure-Based Biologiche, Farmaceutiche Biomaterials e Ambientali, University of Messina, 98168 Messina, Italy; [email protected] 4 INSTM, University of Messina, 98168 Messina, Italy Simone Adorinni 1, Maria C. Cringoli 1,2, Siglinda Perathoner 3,4, Paolo Fornasiero 1,2,5 and Silvia Marchesan 1,2,* 5 Istituto di Chimica dei Composti Organometallici, Consiglio Nazionale delle Ricerche (ICCOM-CNR), 34127 Trieste, Italy 1 *ChemicalCorrespondence: and Pharmaceutical [email protected] Sciences Department, University of Trieste, 34127 Trieste, Italy; [email protected] (S.A.); [email protected] (M.C.C.); [email protected] (P.F.) 2 INSTM, University of Trieste, 34127 Trieste, Italy 3 Abstract:DipartimentoThe di Scienze family Chimiche, of carbon Biologiche, nanostructures Farmaceutiche e Ambientali, comprises University several of members,Messina, such as fullerenes, nano- 98168 Messina, Italy; [email protected] 4 onions,INSTM, University nanodots, of Messina, nanodiamonds, 98168 Messina, Italy nanohorns, nanotubes, and graphene-based materials. Their 5 uniqueIstituto di electronicChimica dei Composti properties Organometallici, have attracted Consiglio Nazionale great interest delle Ricerche for (ICCOM-CNR), their highly innovative potential in 34127 Trieste, Italy * nanomedicine.Correspondence: [email protected] However, their hydrophobic nature often requires organic solvents for their dis- persibility and processing. In this review, we describe the green approaches that have been developed Abstract:to produce The family and of functionalize carbon nanostructures carbon comprises nanomaterials several members, for biomedical such as fullerenes, applications, nano- with a special focus onions, nanodots, nanodiamonds, nanohorns, nanotubes, and graphene-based materials. Their uniqueon the electronic very latest properties reports. have attracted great interest for their highly innovative potential in nanomedicine. However, their hydrophobic nature often requires organic solvents for their dispers- ibilityKeywords: and processing.carbon In this nanostructures; review, we describe graphene; the green carbon approaches nanotubes; that have been carbon developed nanodots; nanodiamonds; tonanomaterials; produce and functionalize biomaterials carbon nanomaterials for biomedical applications, with a special focus on the very latest reports. Citation: Adorinni, S.; Cringoli, M.C.; Perathoner, S.; Fornasiero, P.; Keywords: carbon nanostructures; graphene; carbon nanotubes; carbon nanodots; nanodiamonds; nanomaterials; biomaterials Marchesan, S. Green Approaches to Citation: Adorinni, S.; 1. Introduction Carbon Nanostructure-Based Cringoli, M.C.; Perathoner, S.; Biomaterials.Fornasiero,Appl. P.; Marchesan, Sci. 2021 ,S.11 Green, 2490. The family of carbon nanostructures (Figure1) comprises of many different members https://doi.org/10.3390/app11062490Approaches to Carbon 1.that Introduction generally share the common feature of being composed of carbon atoms, covalently 2 Nanostructure-Based Biomaterials. boundThe family in a of sp carbonhexagonal nanostructures lattice, (Figur althoughe 1) comprises exceptions of many different exist [members1]. The two-dimensional Appl. Sci. 2021, 11, x. Academic Editor: Greta Varchi that(2D)-sheet generally share of graphene the common can feature be considered of being composed as a universal of carbon buildingatoms, covalently block, which, depending https://doi.org/10.3390/xxxxx boundon how in a sp it2 ishexagonal folded, lattice, can give although rise exceptions to 0D fullerenes exist [1]. The [2 two-dimensional], 1D single-wall (2D)- [3] or multi-wall [4] sheet of graphene can be considered as a universal building block, which, depending on Received:Academic 23 February Editor: Greta 2021 Varchi carbon nanotubes (CNTs), or 2D-graphene-based materials [5]. Other nanostructures how it is folded, can give rise to 0D fullerenes [2], 1D single-wall [3] or multi-wall [4] Accepted: 5 March 2021 comprise nano-onions (CNOs) [6], nanohorns (CNHs) [7], nanocones, and nanodiscs [8]. Received: 23 February 2021 carbon nanotubes (CNTs), or 2D-graphene-based materials [5]. Other nanostructures Published: 11 March 2021 3 Accepted: 5 March 2021 compriseNanodiamonds nano-onions (NDs)(CNOs) differ[6], nanohorns for they (CNHs) contain [7], nanocones, a large and portion nanodiscs of sp[8]. carbon atoms [9]. 3 Published: 10 March 2021 NanodiamondsMore recently, (NDs) carbon differ for dots they have contain acquired a large portion increasing of sp carbon attention atoms [9]. [10 More]. Furthermore, carbon Publisher’s Note: MDPI stays neutral recently,nanostructures carbon dots can have be assembledacquired increasing together attention in superstructures [10]. Furthermore, [11 ]carbon and 3D-materials [12]. with regardPublisher’s to jurisdictional Note: MDPI stays claims neu- in nanostructures can be assembled together in superstructures [11] and 3D-materials [12]. tral with regard to jurisdictional published maps and institutional affil- claims in published maps and institu- iations.tional affiliations. Copyright: © 2021 by the authors. Submitted for possible open access Copyright: © 2021 by the authors. publication under the terms and con- Licenseeditions MDPI, of the Creative Basel, Commons Switzerland. At- This articletribution is (CC an BY) open license access (http://crea- article distributedtivecommons.org/licenses/by/4.0/). under the terms and conditions of the Creative Commons Attribution (CC BY) license (https:// creativecommons.org/licenses/by/ Figure 1. Carbon nanostructures discussed in this review (not to scale). The nano-onion schematic 4.0/). structure is reproduced with permission from [13], copyright ©1995, Elsevier. Appl. Sci. 2021, 11, x. https://doi.org/10.3390/xxxxx www.mdpi.com/journal/applsci Appl. Sci. 2021, 11, 2490. https://doi.org/10.3390/app11062490 https://www.mdpi.com/journal/applsci Appl. Sci. 2021, 11, 2490 2 of 20 Each of these components has its own unique properties related to the specific mor- phology, size, and reactivity. They generally feature very interesting electronic conductivity, high mechanical strength, low density, as well as the ability to undergo chemical func- tionalization to further tune their properties as needed for the intended application. It is thus not surprising that many reviews already exist on their clinical applications [14] in biomedicine [15–17] and, above all, on their potential use in oncology [18], such as innova- tive components in cancer theranostics [19] and cancer therapy [20], thanks to their ability to target the tumor micro-environment [21]. Indeed, the possibility to use them not only as vehicles for drug delivery [22], but also for innovative imaging [23] and biosensing [24], makes them ideal candidates for innovative theranostics [25,26]. Research is also very active on their applications to target diseases other than cancer, such as atherosclerosis [27], and infections [28], including the recent fight against coro- naviruses [29]. Further areas of intense investigation include tissue engineering [30], in particular to reconstruct the heart [31] and to re-establish neural connections [32], due to their demonstrated ability to boost the electrical activity of conductive tissue [33] and stimu- late nerve growth [34]. Finally, there has been increased interest in their electron-conductive abilities, to develop innovative wearable electronics [35]. Interactions between carbon nanomaterials and biomolecules, especially DNA [36] and proteins [37], are the object of many investigations, due to their role in determining the dynamic structure of the biomolecular corona [38], which ultimately affects the response in vivo [39], e.g., the biodistribution [40], the immune response [41], for instance mediated by neutrophils [42], and, thus, the biodegradation [43]. Despite decades of research efforts in these sectors, there are still many concerns regarding carbon nanostructure toxicity [44,45] and immunogenicity [46], also due to the high heterogeneity of this class of materials, which present both unexploited opportunities and unresolved challenges [47] in nanomedicine. In particular, one of the latter regards the large-scale production for mainstream applications [48], considering the current emergency we are facing, in terms of preservation of the environment, especially the development and implementation of green routes for their sustainable production. Therefore, in light of the vastness and complexity of the topic of carbon nanomaterials for biomedical applications, this concise review aims to cover only the most recent advances in the nanomedicine area that describe green chemical routes for their preparation and chemical modifications, in the hope that it will inspire scientists that enter this area towards more environmentally conscious choices for their chemical procedures. 2. Green Routes to Prepare Carbon Nanomaterials for Biomedical Applications In recent years, researchers have been paying
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