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Carbon-Based Nanomaterials 3.0 Edited by Ana María Díez-Pascual Printed Edition of the Special Issue Published in International Journal of Molecular Sciences www.mdpi.com/journal/ijms Carbon-Based Nanomaterials 3.0 Carbon-Based Nanomaterials 3.0 Editor Ana Mar´ıa D´ıez-Pascual MDPI‚Basel‚Beijing‚Wuhan‚Barcelona‚Belgrade‚Manchester‚Tokyo‚Cluj‚Tianjin Editor AnaMar´ıaD´ıez-Pascual AnalyticalChemistry UniversidaddeAlcala´ Madrid Spain EditorialOffice MDPI St. Alban-Anlage66 4052Basel,Switzerland This is a reprint of articles from the Special Issue published online in the open access journal InternationalJournalofMolecularSciences (ISSN 1422-0067) (available at: www.mdpi.com/journal/ ijms/special issues/carbon nano 3). For citation purposes, cite each article independently as indicated on the article page online and as indicatedbelow: LastName, A.A.; LastName, B.B.; LastName, C.C. Article Title. Journal Name Year, Volume Number, PageRange. ISBN978-3-0365-6551-4(Hbk) ISBN978-3-0365-6550-7(PDF) © 2023 by the authors. Articles in this book are Open Access and distributed under the Creative Commons Attribution (CC BY) license, which allows users to download, copy and build upon publishedarticles,aslongastheauthorandpublisherareproperlycredited,whichensuresmaximum disseminationandawiderimpactofourpublications. ThebookasawholeisdistributedbyMDPIunderthetermsandconditionsoftheCreativeCommons licenseCCBY-NC-ND. Contents AbouttheEditor ....................................................................................................................................... vii Prefaceto”Carbon-BasedNanomaterials3.0” . . . . . . . . . . . . . . . . . . . . . . . . . . . . . ix AnaM.D´ıez-Pascual Carbon-BasedNanomaterials3.0 Reprintedfrom: Int. J.Mol. Sci. 2022,23,9321,doi:10.3390/ijms23169321 . . . . . . . . . . . . . . 1 DanielaBala, IuliaMatei,GabrielaIonita, Dragos-ViorelCosma,Marcela-CorinaRosuand MariaStancaetal. Luminescence, Paramagnetic, and Electrochemical Properties of Copper Oxides-Decorated TiO /GrapheneOxideNanocomposites 2 Reprintedfrom: Int. J.Mol. Sci. 2022,23,14703,doi:10.3390/ijms232314703 . . . . . . . . . . . . . 5 Thi-HoaLe,Ji-HyeonKimandSang-JoonPark “Turnon”FluorescenceSensorofGlutathioneBasedonInnerFilterEffectofCo-DopedCarbon Dot/GoldNanoparticleComposites Reprintedfrom: Int. J.Mol. Sci. 2021,23,190,doi:10.3390/ijms23010190 . . . . . . . . . . . . . . . 17 Emo˝ke Sikora, Ga´bor Mura´nszky, Ferenc Krista´ly, Be´la Fiser, La´szlo´ Farkas and Be´la Viskolczetal. Development of Palladium and Platinum Decorated Granulated Carbon Nanocomposites for CatalyticChlorateElimination Reprintedfrom: Int. J.Mol. Sci. 2022,23,10514,doi:10.3390/ijms231810514 . . . . . . . . . . . . . 29 Joon-HyukBang,Byeong-HoonLee,Young-ChulChoi,Hye-MinLeeandByung-JooKim A Study on Superior Mesoporous Activated Carbons for Ultra Power Density Supercapacitorfrom BiomassPrecursors Reprintedfrom: Int. J.Mol. Sci. 2022,23,8537,doi:10.3390/ijms23158537 . . . . . . . . . . . . . . 43 VitoDespojaandLeonardoMarusˇic´ PredictionofStrongTransversals(TE)Exciton–PolaritonsinC60ThinCrystallineFilms Reprintedfrom: Int. J.Mol. Sci. 2022,23,6943,doi:10.3390/ijms23136943 . . . . . . . . . . . . . . 57 Rene Mary Amirtha, Hao-Huan Hsu, Mohamed M. Abdelaal, Ammaiyappan Anbunathan,Saad G.MohamedandChun-ChenYangetal. Constructing a Carbon-Encapsulated Carbon Composite Material with Hierarchically Porous ArchitecturesforEfficientCapacitiveStorageinOrganicSupercapacitors Reprintedfrom: Int. J.Mol. Sci. 2022,23,6774,doi:10.3390/ijms23126774 . . . . . . . . . . . . . . 77 TingSun,XianLi,XiaochuanJin,ZiyiWu,XiachaoChenandJieqiongQiu FunctionofGrapheneOxideasthe“Nanoquencher”forHg2+ DetectionUsinganExonucleaseI- AssistedBiosensor Reprintedfrom: Int. J.Mol. Sci. 2022,23,6326,doi:10.3390/ijms23116326 . . . . . . . . . . . . . . 89 TomasPlachy,ErikaKutalkova,DavidSkodaandPavlinaHolcapkova TransformationofCelluloseviaTwo-StepCarbonizationtoConductingCarbonaceousParticles andTheirOutstandingElectrorheologicalPerformance Reprintedfrom: Int. J.Mol. Sci. 2022,23,5477,doi:10.3390/ijms23105477 . . . . . . . . . . . . . . 103 v JoonwonBae,GyoEunGu,YeonJuKwon,JeaUkLeeandJin-YongHong Functionalization of Tailored Porous Carbon Monolith for Decontamination of Radioactive Substances Reprintedfrom: Int. J.Mol. Sci. 2022,23,5116,doi:10.3390/ijms23095116 . . . . . . . . . . . . . . 117 Mo´nica Canales, Juan Manuel Ramı´rez-de-Arellano, Juan Salvador Arellano and Luis FernandoMagan˜a Ab Initio Study of the Interaction of a Graphene Surface Decorated with a Metal-Doped C 30 withCarbonMonoxide,CarbonDioxide,Methane,andOzone Reprintedfrom: Int. J.Mol. Sci. 2022,23,4933,doi:10.3390/ijms23094933 . . . . . . . . . . . . . . 131 Leonardo Marusˇic´, Ana Kalinic´, Ivan Radovic´, Josip Jakovac, Zoran L. Misˇkovic´ and Vito Despoja ResolvingtheMechanismofAcousticPlasmonInstabilityinGrapheneDopedbyAlkaliMetals Reprintedfrom: Int. J.Mol. Sci. 2022,23,4770,doi:10.3390/ijms23094770 . . . . . . . . . . . . . . 149 Wen-ShuoKuo,Yen-SungLin,Ping-ChingWu,Chia-YuanChang,Jiu-YaoWangandPei-Chi Chenetal. Two-Photon–Near Infrared-II Antimicrobial Graphene-Nanoagent for Ultraviolet–Near InfraredImagingandPhotoinactivation Reprintedfrom: Int. J.Mol. Sci. 2022,23,3230,doi:10.3390/ijms23063230 . . . . . . . . . . . . . . 165 Viritpon Srimaneepong, Hans Erling Skallevold, Zohaib Khurshid, Muhammad Sohail Zafar,DineshRokayaandJanakSapkota GrapheneforAntimicrobialandCoatingApplication Reprintedfrom: Int. J.Mol. Sci. 2022,23,499,doi:10.3390/ijms23010499 . . . . . . . . . . . . . . . 177 Manuel A. Valde´s-Madrigal, Fernando Montejo-Alvaro, Amelia S. Cernas-Ruiz, Hugo Rojas-Cha´vez,RamonRoma´n-DovalandHeribertoCruz-Martinezetal. Role of Defect Engineering and Surface Functionalization in the Design of Carbon Nanotube-BasedNitrogenOxideSensors Reprintedfrom: Int. J.Mol. Sci. 2021,22,12968,doi:10.3390/ijms222312968 . . . . . . . . . . . . . 195 vi About the Editor AnaMar´ıaDı´ez-Pascual Ana Maria Diez-Pascual graduated in Chemistry in 2001 (awarded Extraordinary Prize) at the Complutense University (Madrid, Spain), where she completed her Ph.D. (2002–2005) on dynamic and equilibrium properties of fluid interfaces under the supervision of Prof. Rubio. In 2005, she worked at the Max Planck Institute of Colloids and Interfaces (Germany) with Prof. Miller on the rheological characterization of water-soluble polymers. During 2006–2008, she was a postdoctoral researcher at the Physical Chemistry Institute of the RWTH-Aachen University (Germany), where she worked on the layer-by-layer assembly of polyelectrolyte multilayers onto thermoresponsive microgels. Then,shemovedtotheInstituteofPolymerScienceandTechnology(Madrid,Spain)and participated in a Canada–Spain joint project to develop carbon nanotube (CNT)-reinforced epoxy and polyetheretherketone composites for transport applications. Currently, she is a full professor at Alcala University (Madrid, Spain) focused on the development of polymer/nanofiller systems for biomedical applications. She has published over 200 SCI articles (97% in Q1 journals). She has an H-index of 43 and more than 4000 total citations. She has published 21 book chapters, 2 monographies, and edited 3 books, and is the first author of an international patent. She has been invited to impart seminars at prestigious international research centers (i.e., Max Planck in Germany, NRC in Canada, School of Materials in Manchester, U.K.). She was awarded the TR35 2012prizebytheMassachusettsTechnologicalInstitute(MIT)forherinnovativeworkinthefieldof nanotechnology. SheismemberoftheYoungAcademyofSpain. vii Preface to ”Carbon-Based Nanomaterials 3.0” ThisSpecialIssue, withacollectionof12originalcontributionsand2literaturereviews, offers selectexamplesofthesurfacemodificationsofcarbonnanomaterialsthatadapttheirphysicochemical properties, as well as their applications in a variety of fields, such as supercapacitors, sensors, antimicrobialcoatings,bioimaging,decontamination,andsoforth. AnaMar´ıaDı´ez-Pascual Editor ix International Journal o f Molecular Sciences Editorial Carbon-Based Nanomaterials 3.0 AnaM.Díez-Pascual UniversidaddeAlcalá,FacultaddeCiencias,DepartamentodeQuímicaAnalítica,QuímicaFísicaeIngeniería Química,Ctra.Madrid-BarcelonaKm.33.6,28805AlcaládeHenares,Madrid,Spain;[email protected] Carbon-basednanomaterialsarecurrentlyattractingalotofinterestinmanyfields, ranging from medicine and biotechnology to electronics, energy storage, and sensing applications [1,2]. They show a variety of shapes, from 0D fullerenes, nanodiamonds, andquantumdots(QDs)to1Dcarbonnanotubes(CNTs),and2Dgraphene(G)andits derivativesgrapheneoxide(GO)andreducedgrapheneoxide(rGO)[3]. Furthermore,new carbon-basednanomaterialsarecurrentlyunderinvestigation,suchasmutatedgraphene- likenanomaterials,whichhavebeenfoundtobeveryeffectivefortheremovaloforganic pollutantsfromwastewater[4],aswell3Dcarbonmonolithics,whichhavegreatpotential forthedecontaminationofradioactivesubstances[5]. One characteristic of all carbon nanomaterials is the possibility of functionalizing themthroughnon-covalentandcovalentmethods[6,7], whichgenerallymodifiestheir hydrophilic, electronic, optical, and mechanical properties. Non-covalent approaches are attained via π–π stacking, electrostatic forces, and Van der Waals forces. On the otherhand,covalentfunctionalizationcanbeperformedviasimpleoxidation,leadingto oxygen-containinggroupssuitableforreactingwithfunctionalgroupsofothermolecules orpolymers. ThisSpecialIssue“Carbon-BasedNanomaterials3.0”,withacollectionof 10 original contributions and 2 literature reviews, offers select examples of the surface modificationsofcarbonnanomaterialsthatadapttheirphysicochemicalproperties,aswell astheirapplicationsinavarietyoffields,suchassupercapacitors,sensors,antimicrobial coatings,bioimaging,decontamination,andsoforth. Withanenlargedglobalfocusontacklingthechallengesofenvironmentalpollution, Citation:Díez-Pascual,A.M. the interest in novel energy devices as an alternative to petroleum-based ones has also Carbon-BasedNanomaterials3.0.Int. increased. In this regard, supercapacitors can be designed for use in environmentally J.Mol.Sci.2022,23,9321. https:// friendly vehicles and new renewable energy; however, the limitation of a low energy doi.org/10.3390/ijms23169321 densityremainsachallenge[8]. Tofurtherincreasethepowerdensityofsupercapacitors, Received:9August2022 mesoporous carbon nanomaterials can be used. However, activated carbons with high Accepted:17August2022 mesoporevolumesgeneratedviaphysicalactivationarenoteconomicallyviable. Thus, Published:18August2022 todevelopcost-effectivehigh-performancesupercapacitorswithhighenergyandpower densities,thepreparationofnovelmesoporousactivatedcarbonsshouldbeinvestigated. Publisher’sNote:MDPIstaysneutral Inthisregard,Bangetal.[9]haverecentlysynthesizedakenaf-derivedactivatedcarbon withregardtojurisdictionalclaimsin (KAC)forahigh-powerdensitysupercapacitorviaphosphoricacidactivation. Kenafwas publishedmapsandinstitutionalaffil- chosenastheprecursorduetoitshighproductivity,andphosphoricacidactivationwas iations. appliedtocreateahighspecificsurfaceareaandadvancedmesoporousstructure. The pore-growth mechanism for KAC through phosphoric acid activation was explored by analyzingthetexturalpropertiesandcrystalstructures. Theelectrochemicalpropertiesof Copyright: © 2022 by the author. KACwerecomparedwithcommercialactivatedcarbon,andanimprovementwasfound Licensee MDPI, Basel, Switzerland. bothinthespecificcapacitanceandtheion-diffusionresistance. Mesoporecontrolofthe This article is an open access article electrodematerialiscrucialinimprovingthesupercapacitorresistanceandoutput. distributed under the terms and Hierarchicalporousactivatedcarbon(HPAC)isanotherinterestingactivematerialfor conditionsoftheCreativeCommons supercapacitorsduetoitshugespecificsurfaceare. Preparingelectrodeswithhigh-mass Attribution(CCBY)license(https:// loadingisinterestinginprovidinghightotalcapacitancesandgravimetricorvolumetric creativecommons.org/licenses/by/ energydensities[10]. Therefore,developinganHPACthatincreasesthemassloadingof 4.0/). 1 Int.J.Mol.Sci.2022,23,9321 theresultingelectrodeishighlydesirable. Inthisregard,Amirthaetal.[11]prepareda novelhydrogel-derivedencapsulatedH-HPAC(H@H)compositematerial,withreduced specificsurfaceareaandporeparametersbutincreasedproportionsofnitrogenspecies. Thefree-standingandflexibleH@Helectrodesshowedremarkablereversiblecapacitance, ratecapability,andcyclingstabilityandarealsopromisingelectrodematerialsforother energystoragefieldssuchasmetal–ioncapacitors. In another study, a novel carbonaceous material was prepared from cellulose car- bonizedviatwo-steps—hydrothermalandthermalcarbonization,inorder—withoutany chemicals[12],givinghighyieldsafteratreatmentat600 Cunderaninertatmosphere. ◦ This led to nanospheres with increased specific surface areas, as confirmed by SEM, FTIR,X-raydiffraction,andRamanspectroscopy,aswellasenhancedconductivity. The nanosphereswereusedasadispersedphaseinelectrorheologicalfluids,displayingexcep- tionalelectrorheologicaleffects,considerablysurpassingrecentstate-of-the-artfindings. Thesenewcarbonaceousparticlespreparedfromrenewablecellulosehavefurtherpotential tobeutilizedinmanyotherapplicationsthatrequireconductingcarbonaceousstructures withhighspecificsurfaceareasuchasadsorption,catalyst,filtration,andenergystorage, tomentionbutafew. GOiswellknownforitsoutstandingfluorescencequenchingcapability. Sunetal.[13] preparedawater-solublepositivelychargedgrapheneoxidebygraftingpolyetherimide ontoGOnanosheetsviaacarbodiimidereaction. ComparedwithconventionalGO,the fluorescencequenchingabilityoftheDNAstrandofthenovelpositivelychargedonewas significantly improved via an additional electrostatic interaction. The DNA probe was almostcompletelyquenchedforconcentrationsofthepositivelychargedGOaslowas 0.1µg/mL.ThisquenchingabilitywasusedtodevelopasensorforHg2+detection,leading toalinearconcentrationrangeof0–250nM,withalimitofdetectionof3.93nM,anditwas successfullyappliedtorealsamplesofpondwater,leadingtorecoveriesintherangefrom 99.6%to101.1%. Basedonthefluorescencequenchingabilityofnitrogen-andphosphorous-dopedcarbon dots,asimpleandselectivesensorforglutathionedetectionwasalsodeveloped[14].There- ductantpotentialofthedopedcarbondotswasusedtosynthesizeAuNPsandtosubsequently formcomposites,whichwerecharacterizedviaspectroscopicandmicroscopictechniques, includingelectrophoreticlightscatteringandXRD.Theoverlapofthefluorescenceemission spectrumofthedopedcarbondotsandtheabsorptionspectrumofAuNPsresultedinan effectiveinnerfiltereffectinthecompositematerial,leadingtoaquenchingofthefluorescence intensity.InthepresenceofGSH,thefluorescenceintensityofthecompositewasrecovered, leadingtoasensingmethodwithalimitofdetectionof0.1µM. Nitrogen-dopedaminoacid-functionalizedGQDsshowenhancedphotoluminescence and photostability and lead to the generation of reactive oxygen species through two- photonphotodynamictherapy(PDT)[15]. Thisamino-N-GQDscanbeusedastwo-photon contrastprobestotrailandlocalizeanalytesinin-depthtwo-photonimagingexecutedina biologicalenvironmentalongwithtwo-photonPDTtoeliminateinfectiousormultidrug- resistantmicrobes. Nitrogenoxides(NOx)areamongsttheforemostatmosphericpollutants;hence,it isimperativetoscreenanddetecttheirpresenceintheatmosphere. Forsuchapurpose, low-dimensionalcarbonstructureshavebeenbroadlyusedasNOxsensors. Inparticular, CNTs have been applied for sensing toxic gases due to their high specific surface area andexcellentmechanicalproperties. EventhoughpristineCNTshaveshownpromising performanceforNOxdetection,severalstrategieshavebeendevelopedsuchassurface functionalization and defect engineering to expand the NOx-sensing ability of pristine CNT-basedsensors. Inthisregard,thesurfacemodificationapproachesusedintherecent decadetomodifythesensitivityandtheselectivityofCNTstoNOxhaverecentlybeen reviewed[16]. OtheratmosphericcontaminantsthatthreatentheenvironmentandlifeincludeCO, CO ,CH ,andO . Canalesetal.[17]haveexploredtheuseofsmallfullerenessuchas 2 4 3 2

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