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Block Copolymers polymers Review ReviewBlock Copolymers: Synthesis, Self-Assembly, andBlock Applications Copolymers: Synthesis, Self-Assembly, and Applications Hongbo Feng 1, Xinyi Lu 1, Weiyu Wang 2, Nam-Goo Kang 1 and Jimmy W. Mays 1,3,* Hongbo1 Department Feng 1of, XinyiChemistry, Lu 1, University Weiyu Wang of Tennesse2, Nam-Gooe, Knoxville, Kang TN1 and 37996, Jimmy USA;W. [email protected] Mays 1,3,* (H.F.); [email protected] (X.L.); [email protected] (N.-G.K.) 1 Department of Chemistry, University of Tennessee, Knoxville, TN 37996, USA; [email protected] (H.F.); 2 Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, TN 37830, USA; [email protected] (X.L.); [email protected] (N.-G.K.) [email protected] 2 Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, TN 37830, USA; 3 Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN 37830, USA [email protected] * Correspondence: [email protected]; Tel.: +1-865-974-0747 3 Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN 37830, USA *Received:Correspondence: 19 September; [email protected]; Accepted: 3 October Tel.: 2017; +1-865-974-0747 Published: 9 October 2017 Received: 19 September 2017; Accepted: 3 October 2017; Published: 9 October 2017 Abstract: Research on block copolymers (BCPs) has played a critical role in the development of Abstract:polymer chemistry,Research with on block numerous copolymers pivotal (BCPs) contributions has played that have a critical advanced role in our the ability development to prepare, of polymercharacterize, chemistry, theoretically with numerous model, and pivotal technologically contributions exploit that havethis class advanced of materials our ability in a tomyriad prepare, of wayscharacterize, in the fields theoretically of chemistry, model, physics, and technologicallymaterial sciences, exploit and biological this class and of materials medical sciences. in a myriad The breathtakingof ways in the progress fields of has chemistry, been driven physics, by the material advancement sciences, in experimental and biological techniques and medical enabling sciences. the Thesynthesis breathtaking and characterization progress has been of a driven wide byrange the advancementof block copolymers in experimental with tailored techniques composition, enabling architectures,the synthesis andand characterizationproperties. In this of a review, wide range we ofbriefly block discussed copolymers the with recent tailored progress composition, in BCP synthesis,architectures, followed and properties. by a discussion In this review,of the fundamen we brieflytals discussed of self-assembly the recent progressof BCPs inalong BCP with synthesis, their applications.followed by a discussion of the fundamentals of self-assembly of BCPs along with their applications. Keywords: block copolymers; synthesis; self-assembly; applications 1. Introduction Block copolymers (BCPs) are a specificspecific class of copolymers, in which the chemically distinct monomer units units are are grouped grouped in in discrete discrete blocks blocks along along the the polymer polymer chain chain [1]. [ 1Figure]. Figure 1 illustrates1 illustrates a few a offew the of many the many architectures architectures of BCPs, of which BCPs, can which be conf canigured be configured into linear, into branched linear, branched (graft and (graft star), and cyclicstar), andmolecular cyclic molecular architectures. architectures. Thanks to Thanks the advancement to the advancement of polymer of polymer synthetic synthetic strategies strategies and techniques,and techniques, e.g., e.g.,controlled controlled polymerization polymerization techniques techniques along along with with facile facile post-polymerizationpost-polymerization functionalization, BCPs BCPs with precisely controlled molecular weights and defineddefined macromolecular architectures cancan be be prepared prepared [2 –[2–8].8]. The The extraordinary extraordinary structural structural and and compositional compositional versatility versatility of BCPs of BCPshas facilitated has facilitated an explosion an explosion in the in the discovery discovery and an implementationd implementation of of innovative innovative synthetic synthetic strategiesstrategies capable of generating generating previously previously unattainable unattainable levels levels of of man-made man-made architectural architectural complexity. complexity. Linear block terpolymers "Comb" graft copolymers "Miktoarm" star terpolymers Cyclic block terpolymers Figure 1. Representative architectures of linear block terpolymers, “comb” graft polymers, miktoarm star terpolymers, and cyclic block terpolymers. Polymers 2017, 9, 494; doi:10.3390/polym9100494 www.mdpi.com/journal/polymers Polymers 2017, 9, 494; doi:10.3390/polym9100494 www.mdpi.com/journal/polymers Polymers 2017, 9, 494 2 of 31 Polymers 2017, 9, 494 2 of 31 One of the ubiquitous features of BCPs is their ability to form a plethora of nanoscale ordered structures.One of By the manipulating ubiquitous features the molecular of BCPs is para theirmeters ability such to form as athe plethora Flory-Huggins of nanoscale interaction ordered structures.parameter By(χ), manipulating the degree of the polymerization molecular parameters (N), and such the volume as the Flory-Huggins fraction (f), various interaction morphologies parameter (includingχ), the degree spherical, of polymerization cylindrical, lamellar, (N), and and the others volume have fraction been ( frevealed), various both morphologies experimentally including and spherical,theoretically cylindrical, [9,10]. lamellar,Furthermore, and others recent have studies been revealed have bothdemonstrated experimentally that andthetheoretically macromolecular [9,10]. Furthermore,architecture is recent another studies key factor have demonstratedin controlling both that thethe macromolecularresulting morphologies architecture and their is another extent key of factorlong range in controlling order [11]. both Due the to resulting these fascinating morphologies features, and theirresearch extent on ofBCPs long has range long order been [11 a]. popular Due to thesetopic worldwide. fascinating features, Figure 2 research shows the on number BCPs has of long publ beenications a popular with the topic topic worldwide. “block copolymer” Figure2 shows over the numberpast five of decades. publications with the topic “block copolymer” over the past five decades. 4500 4000 3500 3000 2500 2000 1500 1000 Number of Publications 500 0 1960 1970 1980 1990 2000 2010 Year Figure 2. The number of publications with block copolymercopolymer as topic against year. The data were obtained from Web ofof ScienceScience (2017(2017 ClarivateClarivate Analytics).Analytics). In addition to the academic interest in BCPs, the scope of applications for BCPs has been rapidly expanding toto the the fields fields of advancedof advanced materials materials (e.g., thermoplastic (e.g., thermoplastic elastomers), elasto drugmers), delivery, drug patterning, delivery, porouspatterning, materials, porous and materials, many others and overmany the others last twoover decades the last [12 two]. Thermoplastic decades [12]. elastomers Thermoplastic take advantageelastomers take of the advantage combination of the of combination rubbery segments of rubbery and segments rigid segments and rigid within segments block within copolymers. block Drugcopolymers. encapsulation Drug andencapsulation delivery are and facilitated delivery by theare amphiphilicityfacilitated by of the block amphiphilicity copolymers in of solution. block Thecopolymers application in solution. of block copolymersThe application in both of theblock soft copolymers lithography in and both synthesis the soft of porouslithography materials and issynthesis based on of the porous various materials nanoscale is based morphologies on the various induced nanoscale by self-assembly. morphologies Each of induced the applications by self- mentionedassembly. Each above of willthe applications be elaborated mentioned on in the mainabove text. will be elaborated on in the main text. This reviewreview briefly briefly covers covers the the recent recent breathtaking breathta progressking progress in the synthesis,in the synthesis, self-assembly self-assembly behavior, andbehavior, applications and applications of BCPs. Section of BCPs.2 briefly Section describes 2 briefly the syntheticdescribes strategiesthe synthetic for the strategies preparation for the of BCPs.preparation Section of3 BCPs. discusses Section BCP 3 self-assemblydiscusses BCP in self-assembly bulk and in solution.in bulk and Section in solution.4 presents Section several 4 presents major applicationsseveral major of applications BCPs in thermoplastic of BCPs in elastomer,thermoplastic drug elastomer, delivery, softdrug lithography, delivery, soft and lithography, porous material and applications.porous material The applications. conclusions andThe futureconclusions perspectives and future of BCP perspectives research are of presentedBCP research in the are last presented section. Wein the hope last that section. this reviewWe hope will that attract this review emerging will researchers attract emerging to this fieldresearchers and advance to this thefield understanding and advance andthe understanding utilization of the and fascinating utilization BCP of the systems. fascinating BCP systems. 2. Synthesis of BCPs SignificantSignificant work has been focused on the synthesissynthesis of BCPs withwith structuralstructural andand compositioncomposition
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