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materials Review Developing Nanostructured Ti Alloys for Innovative Implantable Medical Devices Ruslan Z. Valiev 1,2, *, Egor A. Prokofiev 2 , Nikita A. Kazarinov 2 , Georgy I. Raab 1 , Timur B. Minasov 3 and Josef Stráský 4 1 Institute of Physics of Advanced Materials, Ufa State Aviation Technical University, 12 K. Marx street, 450008 Ufa, Russia; giraab@mail.ru 2 Laboratory of Mechanics of Advanced Bulk Nanomaterials, Saint Petersburg State University, Universitetskiy prospekt 28, Peterhof, 198504 St. Petersburg, Russia; egpro@mail.ru (E.A.P.); n.kazarinov@spbu.ru (N.A.K.) 3 Department of Traumatology and Orthopedics, Bashkir State Medical University, 3 Lenin street, 450008 Ufa, Russia; m004@yandex.ru 4 Department of Physics of Materials, Charles University, Ke Karlovu 3, 121 16 Prague, Czech Republic; josef.strasky@gmail.com * Correspondence: ruslan.valiev@ugatu.su Received: 31 October 2019; Accepted: 14 February 2020; Published: 21 February 2020 Abstract: Recent years have witnessed much progress in medical device manufacturing and the needs of the medical industry urges modern nanomaterials science to develop novel approaches for improving the properties of existing biomaterials. One of the ways to enhance the material properties is their nanostructuring by using severe plastic deformation (SPD) techniques. For medical devices, such properties include increased strength and fatigue life, and this determines nanostructured Ti and Ti alloys to be an excellent choice for the engineering of implants with improved design for orthopedics and dentistry. Various reported studies conducted in this field enable the fabrication of medical devices with enhanced functionality. This paper reviews recent development in the field of nanostructured Ti-based materials and provides examples of the use of ultra-fine grained Ti alloys in medicine. Keywords: nanostructured Ti alloys; severe plastic deformation; enhanced strength and fatigue life; medical implants with improved design; shape-memory NiTi alloy; functionality 1. Introduction Presently, Ti and its alloys represent the top choice when a combination of high strength, light weight, and affordable cost are required, such as in the area of medical device manufacturing. However, the clinical demands for implantable medical devices are growing rapidly, and nowadays new Ti alloys are being investigated in terms of their chemical composition optimization, manufacturing processes and modification of surface to meet the appropriate medical standards and comply with regulation [1,2]. One possibility to design and manufacture new materials with enhanced properties focuses on nanostructuring of metallic materials using the so-called severe plastic deformation (SPD) techniques, which have become a cutting edge and promising area in materials science and engineering [3,4]. Different SPD techniques are applied to refine grains in metallic materials to below micrometer range or even to the nanosized range. SPD techniques are also efficient for the formation of nanoclusters and nanoprecipitates of secondary phases, enhancing the mechanical and functional properties of the materials [4,5]. A whole variety of SPD techniques have been developed and put forward to provide very high strains (ε > 5) under high applied pressure, such as accumulative roll bonding Materials 2020, 13, 967; doi:10.3390/ma13040967 www.mdpi.com/journal/materials
Materials 2020, 13, 967 2 of 16 (ARB), including multiple forging, twist extrusion, and others [6–8]. However, equal channel angular pressing (ECAP) and high pressure torsion (HPT), introduced already in the pioneering works [3], remain the most used methods for the production of ultrafine-grained (UFG) materials. Principles of these techniques, developed devices and microstructure evolution during processing steps have been thoroughly reviewed in numerous studies [3–7,9,10]. Recently, these deformation techniques have been further upgraded for practical application [11,12]. Nanostructuring of metallic materials increases material strength due to work hardening and grain refinement [13,14], consequently, fatigue life can be also significantly increased by microstructure refinement [15]. Understanding material processing by SPD techniques is essential for designing of medical devices with improved functionality as it not only improves mechanical properties but also affects corrosion and biomedical properties [16–18]. Improved strength and enhanced biomedical response of a nanostructured material can be efficiently used in dental implants; a stent of such permanent implant manufactured from nanostructured Ti can be significantly smaller due to the increased strength and therefore less harmful for a patient [19]. Recently, materials scientists have been exploring possibilities of improved interaction of nanostructured materials with body tissues, for instance bones. In this respect, surface modifications of bulk nanomaterials demonstrate encouraging results [17,18,20,21]. These improvements provide the possibility for development and design of implantable medical devices that perform better and provide improved functionality in comparison to their counterparts manufactured from common coarse-grained materials. This review article outlines the progress in engineering of advanced nanostructured Ti alloys and medical implants/devices manufactured from those advanced materials. 2. SPD Processing of Nanostructured Titanium Materials 2.1. Commercially Pure Ti The first studies devoted to Ti-based materials potentially applicable in medicine were applied to commercial purity titanium (CP Ti) due to its high biocompatibility with living tissues [22]. Unparalleled biocompatibility of Ti was the main interest of many clinical studies of medical devices and tools applied in traumatology, orthopedics, and dentistry. Unfortunately, CP Ti is characterized by reduced strength when compared to other metallic materials used in biomedical devices such as steels or cobalt-based alloys. Achieving higher strength level is possible by alloying or thermo-mechanical processing, but then the Ti-based materials usually lose their biometric response or fatigue performance. Therefore, SPD processing was considered as an alternative strategy proving that nanostructuring of CP Ti may become a novel approach to improve the mechanical properties of this material to achieve its high-performance [13,17,19,20,23]. Apart from enhancing mechanical properties, this strategy is also advantageous in improving the biological response of the surface of the CP titanium based products [18,20]. The first results on nanostructured CP Ti Grade 4 (O–0.34%, Fe–0.3%, C–0.052%, N–0.015%, all in wt.%, balance–Ti] were achieved by Valiev et al. aiming on manufacturing rods with significantly enhanced mechanical properties and superior biomedical response for the fabrication of dental implants [19]. The processing route involved equal-channel angular pressing (ECAP) as an SPD technique [9] followed by thermo-mechanical treatment by forging and, finally, drawing. Continuous SPD processing by ECAP-Conform (ECAP-C) and subsequent drawing, was capable of producing rods with the diameter of 7 mm and the length of 3 m with homogeneous ultrafine-grained (UFG) structure along the entire length of the rods [23,24]. Furthermore, ECAP-Conform represents an economical SPD-based fabrication procedure for mass production of ‘nanoTi’. After combined severe plastic deformation and thermo-mechanical processing, the grain size was significantly reduced from 25 µm in the initial Ti rods to 150 nm in the processed material. Figure 1 illustrates the effect of ECAP-C strain on the density of high-angle boundaries (HAB) and mechanical strength of CP Ti Grade 4 [21].
Materials 2020, 13, 967 3 of 16 Materials 2020, 13, 967 3 of 15 Figure1.1.Influence Figure InfluenceofofECAP-C ECAP-Cstrain onon strain (a)(a) grain boundary grain (GB) boundary density, (GB) (b) yield density, strength (b) yield and (c) strength andthe (c) contribution of various strengthening mechanisms [21]. the contribution of various strengthening mechanisms [21]. Table Table11shows showsthe theimproved improvedmechanical mechanicalproperties propertiesofofCP CPTiTiafter afternanostructuring nanostructuringby byECAP ECAPandand subsequent thermomechanical treatment. The strength of the nanostructured titanium subsequent thermomechanical treatment. The strength of the nanostructured titanium is doubled is doubled when compared to the conventional when compared CP titanium. to the conventional CP The increase titanium. Thein increase strength was achievedwas in strength without reduction achieved of without ductility (total elongation to failure is above the limit of 10%), which is otherwise commonly reduction of ductility (total elongation to failure is above the limit of 10%), which is otherwise observed after intensive commonly drawing observed or rolling. after intensive drawing or rolling. Table1.1.Mechanical Table Mechanicalproperties propertiesofofcoarse-grained coarse-grained(CG) (CG)and andnanostructured nanostructuredCP CPGrade Grade44Ti. Ti.Annealed Annealed Ti-6Al-4V ELI (extra low interstitials) alloy for comparison. Ti-6Al-4V ELI (extra low interstitials) alloy for comparison. Fatigue Reduction Fatigue State Processing UTS, MPaUTS, YS, MPa YS, Elongation, Elongation, % Reduction Strength at State Processing Area, % Strength at MPa MPa % Area, % 106 Cycles 106 Cycles 1 Initial CG Ti 700 530 25 52 340 1 Initial CG Ti 700 530 25 52 340 2 2 nanoTinanoTi 1240 1240 1200 1200 1212 42 42 620 620 Annealed Annealed 3 3 Ti-6Al-4V 940 840840 1616 45 45 530 530 Ti-6Al-4V ELI 940 ELI Fatigue tests of conventional and nanostructured CP Ti were conducted in air at room temperaturetests Fatigue of conventional in accordance withand nanostructured ASTM E 466-96 with CP the Ti were conducted loading in airofat20 frequency roomHztemperature and R = 0.1. in accordance Table 1 showswith thatASTM E 466-96 the fatigue with of strength thenanoTi loading frequency [17,24] after of one20million R = 0.1. Hz andcycles Table 1doubled is almost shows that the fatigue strength of nanoTi [17,24] after one million cycles is almost when compared to the conventional CP titanium and even exceeds the fatigue performance of the Ti-doubled when compared to the conventional CP titanium and even exceeds the fatigue performance 6Al-4V alloy [22,25]. Significant enhancement of fatigue properties and improved strength of of the Ti-6Al-4V alloy [22,25]. Significant nanostructuredenhancement Ti allowof usfatigue properties to produce smaller and improved sizes strength of implants andof nanostructured therefore to reduce Tithe allow us to extent of produce smaller sizes of implants a surgical intervention (see also Section 3). and therefore to reduce the extent of a surgical intervention (see also Section CP3).Ti is known for its considerable biocompatibility which results from the presence of the CP Ti is protective known oxide film.for its considerable Titanium dioxide TiO biocompatibility 2 forms naturally which on theresults surfacefrom of CPtheTipresence of the and represents protective oxide film. Titanium dioxide a stable protective layer on that a mineralized TiO 2 forms naturally on the surface of CP Ti and bone matrix can be attached. This film is usually 5–represents a stable 10nmprotective thick andlayer on that a inert, biologically mineralized thus itbone matrixacan prevents be attached. potentially This film negative is usually reaction 5–10nm between the thick and biologically inert, thus it surrounding body environment and the metal [22].prevents a potentially negative reaction between the surrounding body NanoTi environment withand UFG thestructure metal [22]. containing high density of non-equilibrium grain boundaries NanoTi achieved bywith SPDUFG structure is also containing characterized by high density of significantly non-equilibrium increased internal grain energy boundaries achieved of the material [3]. by SPD is also characterized by significantly increased internal energy of This fact may result in considerable change in the morphology of the oxide film on the materialthe material [3]. This fact may result in considerable surface. NanoTi with change in thesurface polished morphology of the exhibits oxide filmbiological improved on the material surface. reaction of theNanoTi surfacewithas polished confirmed surface exhibits by recent improved studies biological in a series reaction of of experiments the surface through as confirmed tests cytocompatibility by recent usingstudies mouse in a series of fibroblast experiments cells [20,26–29].through At the cytocompatibility same time, additional tests using mouse fibroblast improvement cells [20,26–29]. of biomedical propertiesAtof the same time, additional nanostructured titanium improvement can be achieved of biomedical by dedicated properties surface of modifications nanostructuredsuch titanium can be as chemical achieved by dedicated surface etching or bioactive coatings [17,18]. modifications such as chemical etching or bioactive coatings [17,18].
Materials 2020,13, Materials2020, 13,967 967 44 ofof1615 2.2. Titanium Alloys 2.2. Titanium Alloys Two-phase (α + β) titanium alloys such as Ti-6Al-4V and Ti-6Al-7Nb continue to be the most Two-phase (α + β) titanium alloys such as Ti-6Al-4V and Ti-6Al-7Nb continue to be the most important metallic materials in the dental and orthopedic fields due to their excellent mechanical important metallic materials in the dental and orthopedic fields due to their excellent mechanical properties and satisfactory biocompatibility [2,22,30,31]. properties and satisfactory biocompatibility [2,22,30,31]. Several recent studies reported improved mechanical and functional properties of Several recent studies reported improved mechanical and functional properties of nanostructured nanostructured titanium alloys. titanium alloys. Microstructure and mechanical properties of Ti-6Al-4V ELI (extra low interstitial alloys for Microstructure and mechanical properties of Ti-6Al-4V ELI (extra low interstitial alloys for medical medical applications) prepared by SPD are reported in [15,32,33]. Round rods of the two-phase alloy applications) prepared by SPD are reported in [15,32,33]. Round rods of the two-phase alloy with with the diameter of 40 mm (Intrinsic Devices Company, San Francisco, CA, USA) and with chemical the diameter of 40 mm (Intrinsic Devices Company, San Francisco, CA, USA) and with chemical composition: Ti–base, Al–6.0%; V–4.2%; Fe–0.2%; О–0.11%; N–0.0025%; Н–0.002%, С–0.001 (wt.%) composition: Ti–base, Al–6.0%; V–4.2%; Fe–0.2%; O–0.11%; N–0.0025%; H–0.002%, C–0.001% (wt.%) had the grain size of about 8 µm in a cross-section and 20 µm in a longitudinal section. X-ray had the grain size of about 8 µm in a cross-section and 20 µm in a longitudinal section. X-ray diffraction diffraction analysis proved that the volume fractions of α and β phases were approximately 85% and analysis proved that the volume fractions of α and β phases were approximately 85% and 15%, 15%, respectively. 250 mm length rods were processed in two steps. The rods were subjected to ECAP respectively. 250 mm length rods were processed in two steps. The rods were subjected to ECAP via via route Bc at 600 °С and subsequently extruded, altogether with total strain of 4.2 [33]. The extrusion route Bc at 600 ◦ C and subsequently extruded, altogether with total strain of 4.2 [33]. The extrusion steps were carried out at 300 °С with the last pass at room temperature for additional strengthening. steps were carried out at 300 ◦ C with the last pass at room temperature for additional strengthening. The rods with the diameter of 18 mm and length up to 300 mm were produced. The rods were finally The rods with the diameter of 18 mm and length up to 300 mm were produced. The rods were finally annealed in the temperature range from 200 °С to 800 °С for 1 h and subsequently cooled in air. annealed in the temperature range from 200 ◦ C to 800 ◦ C for 1 h and subsequently cooled in air. Transmission electron microscopy (TEM) studies showed that SPD leads to a complex UFG Transmission electron microscopy (TEM) studies showed that SPD leads to a complex UFG structure containing refined grains and subgrains with a mean size of about 300 nm. structure containing refined grains and subgrains with a mean size of about 300 nm. Stress–strain curves for the initial coarse-grained and UFG material shown in Figure 2 Stress–strain curves for the initial coarse-grained and UFG material shown in Figure 2 demonstrate demonstrate that the alloy after grain refinement by SPD underwent significant strengthening. that the alloy after grain refinement by SPD underwent significant strengthening. Tensile elongation of Tensile elongation of the UFG material (curve 2) is reduced from 17% to 9%. Strength/ductility trade the UFG material (curve 2) is reduced from 17% to 9%. Strength/ductility trade off, however, improved off, however, improved after subsequent annealing at 500 °С. The results of tensile tests correspond after subsequent annealing at 500 ◦ C. The results of tensile tests correspond to the measurement of to the measurement of microhardness [32,33]. microhardness [32,33]. Figure 2. Engineering stress−strain tensile curves of the Ti-6Al-4V ELI alloy: coarse-grained material (initial) Figure(1); UFG condition 2. Engineering (2) and UFG stress−strain condition tensile curvesafter annealing of the 500 ◦alloy: at ELI Ti-6Al-4V C (3).coarse-grained material (initial) (1); UFG condition (2) and UFG condition after annealing at 500 °С (3). In accordance with [10], enhancement of the ductility in the UFG material by annealing is clearly associated with a decrease In accordance of internal with [10], elasticof enhancement stress and dislocation the ductility density. in the UFG Simultaneous material by annealing additional is clearly strengthening of the alloy can be explained by the observed decrease in content of metastable associated with a decrease of internal elastic stress and dislocation density. Simultaneous additional β-phase after cooling from strengthening the of the annealing alloy temperature. can be explained by theIts volumedecrease observed fraction in incontent the UFG alloy annealed of metastable at β-phase 500 ◦ afterCcooling can be higher from the than before annealing, annealing temperature.as shown in [10], Its volume due toinquenching fraction fromannealed the UFG alloy the annealing at 500 temperature. Despite no visible particles of any secondary phase, aging °С can be higher than before annealing, as shown in [10], due to quenching from theprocesses might have caused annealing grain boundaryDespite temperature. segregations associated no visible with particles of additional improvement any secondary of the phase, aging properties processes of the might annealed have caused UFG material [34]. grain boundary segregations associated with additional improvement of the properties of the annealed UFG material [34].
Materials 2020, 13, 967 5 of 16 Materials 2020, 13, 967 5 of 15 Finetuning Fine tuningofofmechanical mechanicalproperties propertiesby byannealing annealingafter afterthe theSPD SPDprocessing processingisislimited limitedmainly mainlyby by grain growth occurring at elevated temperatures. Thermal stability of UFG structure grain growth occurring at elevated temperatures. Thermal stability of UFG structure of commercially of commercially pure Ti pure Ti follows follows classical classical grain grain growth growth depending depending on on temperature temperature via via Arrhenius Arrhenius equation equation [35] [35] and and limited to approximately 450 ◦ C [36]. Nanostructured α + β exhibit enhanced thermal stability up to limited to approximately 450 °C [36]. Nanostructured α + β exhibit enhanced thermal stability up to ◦ C [37]. 550°C 550 [37]. Fatigue properties Fatigue properties ofofthe theTi-6Al-4V Ti-6Al-4V ELIELI alloyalloy withwith UFG UFGstructure were investigated. structure High strength were investigated. High and enhanced ductility (1370 MPa and 12%) after SPD processing and subsequent strength and enhanced ductility (1370 МPа and 12%) after SPD processing and subsequent annealing annealing at 500 ◦ C; resulted at 500 °С in an enhancement resulted of fatigue in an enhancement oflimit to 740 fatigue MPa limit after to 740 МPа107after cycles 107incycles comparison to 600 MPa in comparison in to 600 the initial coarse-grained condition (Figure 3) [32]. МPа in the initial coarse-grained condition (Figure 3) [32]. Figure 3. Fatigue test results of initial coarse-grained material and UFG material after annealing at 500 ◦ C,3.1 Fatigue Figure h. test results of initial coarse-grained material and UFG material after annealing at 500 °С, 1 h. The fatigue limit of the Ti-6Al-4V alloy in UFG condition reported in [32] tested by rotating bending The was slightly fatigue limithigher of thethan the values Ti-6Al-4V in [32,38] alloy in UFGproving thatreported condition measuredinfatigue properties [32] tested depend by rotating on the choice of the measurement technique. bending was slightly higher than the values in [32,38] proving that measured fatigue properties depend Achieved results of on the choice show the that high strength measurement can be achieved in UFG Ti-6Al-4V ELI alloy by processing technique. by ECAP and subsequent Achieved results show thermo-mechanical that high strengthtreatment. SelectioninofUFG can be achieved SPD Ti-6Al-4V regimes and ELIadjustment alloy by processing by ECAP and subsequent thermo-mechanical treatment. Selection of SPD regimes us of processing parameters of SPD processing such as temperature, strain rate and strain allow andto manipulateofthe adjustment grain boundary processing parametersstructure of SPD and phase morphology processing in the two-phase such as temperature, UFGand strain rate alloy. As strain the result, allow us to the best combination manipulate the grain of strengthstructure boundary and ductility can bemorphology and phase achieved along with in the the improved two-phase UFG fatigue alloy. Asendurance the result,limit. Enhancement the best combination of of strength strength and ductility and ductilityof the can biomedical be achievedTi-6Al-7Nb along withalloy the was reported improved in another fatigue endurance comprehensive study [39]. limit. Enhancement of In comparison strength to Ti-6Al-4V, and ductility of thethe Ti-6Al-7Nb biomedical alloy Ti-6Al- represents 7Nb alloy wasa better reportedchoice for biomedical in another use duestudy comprehensive to avoiding the toxic vanadium [39]. In comparison [40]. the to Ti-6Al-4V, This study Ti-6Al- shows 7Nb that alloy processing represents by ECAP a better andfor choice consequent biomedicalthermo-mechanical use due to avoidingtreatment the toxic causing vanadium formation [40]. This of UFG structure study shows that results in high strength processing by ECAP (1400andMPa) and ductility consequent (elongation of 10%). thermo-mechanical These achieved treatment causing propertiesof formation areUFG attractive for designing, structure developing results in high and manufacturing strength(1400 of high-performance MPa) and ductility (elongation ofmedical 10%). devicesachieved These and implants. properties are attractive for designing, developing and manufacturing of high- Considering performance medical that vanadium devices and partly also aluminum are rather toxic elements and, and implants. simultaneously, Considering that that reducing vanadiumofand the partly Young’s alsomodulus aluminum is required are ratherfortoxic avoiding elements so-called and, stress-shielding that simultaneously, [39], reducing the development of brandmodulus of the Young’s new biomedical alloysfor is required represents avoidingaso-called current relevant stress- challenge [39], shielding for researchers. A new generation the development of brand of newtitanium alloys must biomedical alloysprovide improved represents strength, a current better relevant biocompatibility, challenge and lower for researchers. A Young’s modulusofthan new generation Ti6Al4V titanium alloy. alloys Current must research provide focuses improved on new strength, alloying better systems, in particular biocompatibility, and lowerTi-Nb and Ti-Mo. Young’s modulus than Ti6Al4V alloy. Current research focuses on Given the new alloying above mentioned systems, requirements, in particular Ti-Nb and Ti-Mo.the interest is drawn to titanium alloys containing high content Givenof the phase,mentioned theβabove because this phase is characterized requirements, the interest byislower drawn Young’s modulus to titanium in the alloys range of containing high content of the β phase, because this phase is characterized by lower Young’s modulus in the range of 55–90 GPa, and thus exhibit lower stress shielding [39,41–43]. Moreover, these Ti alloys are
Materials 2020, 13, 967 6 of 16 Materials 2020, 13, 967 6 of 15 55–90 GPa, and thus exhibit lower stress shielding [39,41–43]. Moreover, these Ti alloys are designed designed to containtoonly contain only non-toxic non-toxic constituentsconstituents such as Nb, suchMo, asZr, Nb,and Mo, Zr,On Ta. andtheTa. On hand, other the other hand, these these materials materials are characterized by comparatively low strength, because the are characterized by comparatively low strength, because the lowest Young’s modulus is obtainedlowest Young’s modulus is obtained only in treated only in solution solutionsingle treated single phase phase β-Ti β-TiAchieving alloys. alloys. Achieving low Young’slow Young’s modulusmodulus and highand high strength strength simultaneously simultaneously is a challenging is a challenging task. Ageing task. Ageing treatments treatments that inducethata fineinduce a fine and and uniform uniform precipitation precipitation of ω and α phaseof ω components and α phaseprovides components provides significant significant strengthening. strengthening. On the other hand, On the other this hand, inevitably this inevitably increases increases the Young’s the Young’s modulus modulus of the alloy [41–43].of the Onlyalloy [41–43].present few studies Only few studiesresults successful presentin successful results in development of thermal treatments without detrimental development of thermal treatments without detrimental effect on some of the relevant mechanical effect on some of the relevant propertiesmechanical [44,45]. properties [44,45]. Advancements Advancements ininthethe areas areas of orthopedics of orthopedics and dentistry and dentistry called forcalled for newforstrategies new strategies development for development of new generation of β-Ti alloys with reduced Young’s modulus of new generation of β-Ti alloys with reduced Young’s modulus and high strength, which would be more and high strength, which suitable would be more for such suitableRecently, applications. for such SPDapplications. processing Recently, has beenSPD processing proposed has been to fabricate proposed to nanocrystalline fabricate β-Ti alloys nanocrystalline β-Ti alloys with high strength, with highofstrength, low modulus elasticitylow andmodulus excellentofbiocompatibility elasticity and excellent [46–51]. biocompatibility [46–51]. Nanostructuring of these alloys leads to improved Nanostructuring of these alloys leads to improved strength due to grain refinement and substructure strength due to grain refinement and In evolution [52]. substructure particular, evolution [52]. Inβ-Ti solution treated particular, Ti15Mosolution treated alloy, which β-Ti Ti15Mo is qualified for alloy, medical which use, is qualified for medical use, can be significantly refined by HPT as demonstrated can be significantly refined by HPT as demonstrated in Figure 4a. Grain size can be decreased well in Figure 4a. Grain size below can100 benm decreased well below [53]. Significant 100 nm [53].apart disadvantage, Significant disadvantage, from limited size of HPTapartsamples, from limited size of is formation HPT samples, is induced of deformation formation ωof deformation phase causing induced ω phaseofcausing sharp increase sharp increase elastic modulus [54]. of elastic modulus Subsequent aging [54]. Subsequent aging of UFG Ti15Mo alloy leads to two-phase α + of UFG Ti15Mo alloy leads to two-phase α + β structure which is also characterized by increased β structure which is also characterized by increased modulus of elasticity modulus [55–57]. of elasticity More promising is [55–57]. More promising using Ti-Nb-Ta-Zr based is usingwhich alloys Ti-Nb-Ta-Zr are less based prone alloys which are less prone to ω phase formation. Ti-29Nb-13Ta-5Zr alloy prepared to ω phase formation. Ti-29Nb-13Ta-5Zr alloy prepared by HPT exhibited increased yield stress from by HPT exhibited increased 550 to 800 yield MPa withstressunchanged from 550 elastic to 800 modulus MPa with[58,59]. unchanged elasticmicrostructure Significant modulus [58,59]. Significant refinement was microstructure refinement recently also achieved was recently also in Ti-35Nb-6Ta-7Zr achieved in biomedical Ti-35Nb-6Ta-7Zr alloy by ECAP (Figure biomedical 4b). alloy by ECAP (Figure 4b). (a) (b) Figure 4. Microstructure Figure 4. Microstructureofof (a)(a) Ti15Mo Ti15Mo alloy alloy prepared prepared by and by HPT HPT(b)and (b) Ti-35Nb-6Ta-7ZZr Ti-35Nb-6Ta-7ZZr alloy alloy prepared prepared by ECAP by ECAP (cross-section). (cross-section). Microstructural refinement Microstructural refinement in in β-Ti alloys can β-Ti alloys can be be also also enhanced enhanced by by multiple multiple twinning twinning and/or and/or martensitic transformation martensitic transformationβ β →→ α’’α” [60]. [60]. The nanocrystalline The nanocrystalline β-Ti alloys β-Ti alloys also display also display excellentexcellent in vitro in vitro biocompatibility biocompatibility as shownas shown by enhanced by enhanced cell cell attachment attachment andand proliferation[48]. proliferation [48].These These novel novel nanocrystalline β-Ti nanocrystalline β-Tialloys alloyshave havehigh chances high to meet chances the challenge to meet of next-generation the challenge implant material of next-generation implant with significant material prospectsprospects with significant in load bearing in loadbiomedical applications. bearing biomedical applications. 2.3. Nanostructured 2.3. Nanostructured NiTi NiTi Shape Shape Memory Memory Alloys Alloys NiTi alloys NiTi alloysexhibit unique exhibit mechanical unique behavior—shape mechanical memory effect behavior—shape (SME)effect memory and superelasticity, (SME) and which arise from a transformation between martensite and austenite phases [61,62]. NiTi alloys superelasticity, which arise from a transformation between martensite and austenite phases are [61,62]. NiTi alloys are important materials which are already used in advanced medical devices due to the above mentioned mechanical properties and, additionally, due to functional properties such as good biocompatibility and corrosion resistance in vivo [61,63]. At the same time, new, advanced
responsible for the shape memory effect [65,66]. During following thermal treatments nanocrystalline (NC) structure can be obtained in NiTi alloys via crystallization process (Figure 5) [64,67]. Nanocrystalline NiTi alloys with grain size about 20 nm demonstrate very high strength up to 2000 MPa [64]. Equal Materials 2020,channel 13, 967 angular pressing is another SPD processing technique applied for producing 7 of 16 uniform UFG structure in bulk NiTi alloys. The ECAP processing of NiTi at 400–450 °C results in formation of UFG structure with grain size of about 200 nm (Figure 5). important UFG materials structure which are already formation leads used in advanced to significant medical devices improvement due to the above of mechanical and mentioned functional mechanical properties and, additionally, due to functional properties such as properties of NiTi-based alloys [64,68–70]. The ultimate tensile strength (UTS) of UFG NiTi alloy good biocompatibility and corrosion attains resistance 1400 in vivois[61,63]. MPa, which 50% higherAt thethan sameintime, CG new, advanced alloys; and theapplications yield stresswill require (YS) enhanced increases after properties (higher strength, higher recovery strain and stress, etc.) of NiTi ECAP from 500 MPa to 1100 MPa (Figure 6a). The functional shape-memory effect of NiTi after ECAP shape memory alloys. During is also improvedthe past two6b). (Figure decades, there hascompletely The maximum been interest in the application recoverable of increases strain εrmax SPD methods fromto6% NiTi (in alloys CG because state) to 9%the formation after ECAP and of nanocrystalline the maximum recoveryand UFGstressstructures σrmax allows reachesenhancing 1120 MPa,mechanical and which is twice functional more than theproperties level ofinCGcomparison alloys (about to coarse 500 MPa) grained materials [69]. UFG [63,64]. structure formation in Ni-rich NiTi alloys HPT processing of NiTi alloys leads to a transformation by ECAP results in an emergence of superelasticity at temperature close from crystalline to thetohuman amorphous body phase. Microstructural changes in deformed NiTi during thermal treatment temperature. Superelasticity in UFG NiTi is characterized by a narrow mechanical hysteresis and are of key interest low as they are residual responsible strain [71]. for the shape memory effect [65,66]. During following thermal treatments nanocrystalline (NC) structure The high-strength NC and canUFGbe obtained in NiTi NiTi alloys alloys with via crystallization improved functionalprocess (Figure 5) characteristics [64,67]. are very Nanocrystalline NiTi alloys with grain size about 20 nm demonstrate promising for medical applications in particular for manufacturing of stents, embolic protection very high strength up to 2000 MPa filters, guide[64]. wires, and other peripheral vascular devices (see Section 4). (a) (b) Figure 5. Microstructure Microstructure of of (a) (a)NC NCand and(b) (b)UFG UFGNiTi NiTialloys alloysprocessed processedby byHPT HPTand andECAP, ECAP,respectively. respectively. Equal channel angular pressing is another SPD processing technique applied for producing uniform UFG structure in bulk NiTi alloys. The ECAP processing of NiTi at 400–450 ◦ C results in formation of UFG structure with grain size of about 200 nm (Figure 5). UFG structure formation leads to significant improvement of mechanical and functional properties of NiTi-based alloys [64,68–70]. The ultimate tensile strength (UTS) of UFG NiTi alloy attains 1400 MPa, which is 50% higher than in CG alloys; and the yield stress (YS) increases after ECAP from 500 MPa to 1100 MPa (Figure 6a). The functional shape-memory effect of NiTi after ECAP is also improved (Figure 6b). The maximum completely recoverable strain εr max increases from 6% (in CG state) to 9% after ECAP and the maximum recovery stress σr max reaches 1120 MPa, which is twice more than the level of CG alloys (about 500 MPa) [69]. UFG structure formation in Ni-rich NiTi alloys by ECAP results in an emergence of superelasticity at temperature close to the human body temperature. Superelasticity in UFG NiTi is characterized by a narrow mechanical hysteresis and low residual strain [71]. The high-strength NC and UFG NiTi alloys with improved functional characteristics are very promising for medical applications in particular for manufacturing of stents, embolic protection filters, guide wires, and other peripheral vascular devices (see Section 4).
Materials 2020, 13, 967 8 of 16 Materials 2020, 13, 967 8 of 15 (a) (b) Mechanical Figure6.6.Mechanical Figure properties properties of NiTi of NiTi alloyalloy in CGincondition CG condition andECAP. and after after ECAP. (a) Engineering (a) Engineering stress– stress–strain strain curves curves for fortests tensile tensile testsstate in CG in CG (1)state (1) and and after afterusing ECAP ECAP using 4 (2), 4 (2), 8 (3) and812(3)(4) and 12 (4)and passes passes (b) and (b) functional properties (ε max and σ max ) as a function of number of ECAP passes [61]. functional properties (εr and σ max r r ) as a function max r of number of ECAP passes [61]. 3.3.Design Designof ofMiniaturized MiniaturizedImplantsImplants Enhanced mechanical Enhanced mechanicalproperties properties of nanostructured of nanostructured metals allowallow metals development of medical development of implants medical with better design, for instance with a more subtle design which is implants with better design, for instance with a more subtle design which is less harmful for less harmful for human body human[17]. Application body [17]. of stronger nanostructured CP Ti instead of common CG Ti, allows for altering the design of devices.ofRecently, Application strongerdetailed computations nanostructured CP Ti were insteadconducted of common to analyze CG Ti, the possible allows geometries for altering the of miniplates for maxillofacial surgery manufactured from nanostructured design of devices. Recently, detailed computations were conducted to analyze the possible Ti [72]. CP Ti of geometries miniplate miniplates specified by ASTMsurgery for maxillofacial F 67, manufactured was considered fromby nanostructured Conmet Company (Moscow, Ti [72]. Russia) as the benchmark for redesigning the product dimensions of CP Ti miniplate specified by ASTM F 67, was considered by Conmet Company (Moscow, Russia) mini-plates manufactured from nanostructured CP Ti. The mechanical properties in a cross-section as the benchmark for redesigning the product dimensions of mini-plates manufactured from of a newly designed plate were calculated with CP nanostructured the Ti. useTheof estimates mechanical of the fatigue performance properties in a cross-sectionlimit for of acoarse-grained newly designed Grade plate4 were CP Ti and nanostructured Grade 4 CP Ti. In practical use, the mini-plates are calculated with the use of estimates of the fatigue performance limit for coarse-grained Grade 4 CP subjected to bending loads, therefore Ti bending strength and nanostructured Grade of 4mini-plates from conventional CP Ti. In practical and nanostructured use, the mini-plates are subjected CPtoTibending was compared. loads, The result bending therefore indicates strength that the plate from nanostructured of mini-plates Ti has significantly from conventional improved bending and nanostructured CP strength Ti was and therefore, compared. Theitresult is clearly advantageous indicates that theoverplatethefrom standard device currently nanostructured Ti hasmanufactured significantly from CG Ti. improved bendingRecently, strengththree-dimensional and therefore, finite it is element models (FEM) over clearly advantageous were the developed standard using CAEcurrently device software (KOMPAS-3D v15, manufactured from CG Ti. ASCON Group, Saint Petersburg, Russia) and then imported into ANSYS Workbench 18.2 Recently, (ANSYS Inc., Canonsburg, PA, three-dimensional USA) finite [73] for element geometry models (FEM)analysis of nanoTiusing were developed dental CAEimplants. software In addition to static (KOMPAS-3D v15,strength, ASCONcalculations Group, Saint of virtual fatigueRussia) Petersburg, testing were carried and then out using imported theANSYS into built-in fatigue module. For all tested models, mesh sensitivity testing was Workbench 18.2 (ANSYS Inc, Canonsburg, Pennsylvania, U.S.A.) [73] for geometry analysis of nanoTi performed in order to obtain mesh-independent results. dental implants. In addition to static strength, calculations of virtual fatigue testing were carried out usingThe the following procedure built-in fatigue was used module. to assess For all tested possible models,ways meshtosensitivity miniaturize the implants. testing The device was performed in with a standard geometry was order to obtain mesh-independent results. assumed to be made from the conventional coarse-grained CP Ti. The model Thewas designed following in a way was procedure to obtain usednearly critical to assess stressways possible state toboth in terms ofthe miniaturize static and fatigue implants. The failure. Afterwards, the same loading was applied to a model with device with a standard geometry was assumed to be made from the conventional coarse-grained reduced dimensions but with CPthe properties of nano CP Ti. Ti. The model was designed in a way to obtain nearly critical stress state both in terms of static and fatigueA failure. one-stage dental implant Afterwards, the samewithloading genericwasgeometry appliedwas to aconsidered model withinreduced the study. The shape dimensions butof the implant is similar to with the properties of nano CP Ti. the implant geometry produced from nano CP Ti by company Timplant s.r.o. (Ostrava, Czech Republic) A one-stage [74]. Figure dental implant with 7generic shows ageometry technical was drawing of the geometry considered of thisThe in the study. nanoimplant shape of with a corresponding numerical model. the implant is similar to the implant geometry produced from nano CP Ti by company Timplant s.r.o. (Ostrava, Czech Republic) [74]. Figure 7 shows a technical drawing of the geometry of this nanoimplant with a corresponding numerical model.
Materials Materials Materials 2020, 2020, 13, 13,13, 2020, 967 967967 9 of 9 9of of 15 1615 (a) (a) (b) (b) (c) (c) Figure Figure 7. 7. 7. Figure Geometry Geometry Geometry of ofof the the the dental dental dental nanoimplant: nanoimplant: (a) (a)(a) nanoimplant: technical technical drawing drawing technical with with drawing dimensions dimensions with in inin dimensions mm;mm; (b) (b)(b) mm; 3D 3D3D model; model; (c) (c) enlarged enlarged FEM FEM mesh. mesh. model; (c) enlarged FEM mesh. TheThe Theapplied applied applied loading scheme loading loading was inspired scheme scheme was by theby was inspired inspired testing by procedures the testing the used in the testing procedures procedures ISOin used used 14801 in the standard. the ISO 14801 ISO 14801 The performed standard. The standard. calculations The performed revealed performed calculations that application calculations revealed revealed that of the nanoTi that application application of allows of the reduction the nanoTi nanoTi allows of the diameter allows reduction reduction ofof the the ofdiameter implant by diameter of at least implant 10%, by at while least 20% 10%, diameter while 20% reduction diameter leads to reduction an unacceptable leads to an decrease unacceptable of implant by at least 10%, while 20% diameter reduction leads to an unacceptable decrease of the decrease device’s of the fatigue of the device’sstrength. device’s fatigue Maximal fatigue strength. principal strength. Maximalstress Maximal zonestress principal principal for thezone stress implant zone with for the for the diameter the implant implant reduced with the with by the diameter diameter 10% loaded reduced by reduced with by 10% a 67.75 10% loaded N force loaded with is shown with aa 67.75 67.75 N in N forceFigure force is 8. is shown shown in in Figure Figure 8. 8. Figure Figure Maximal 8. 8. Figure principal 8. Maximal Maximal stress principal principal for the stress stress forUFG for Ti implant the UFG the UFG with awith Ti implant Ti implant 10%areduced with a 10% diameter 10% reduced reduced and 67.75 diameter diameter and andN 67.75 force. 67.75 NN force. force. 4. Fabrication and Tests of Medical Nanoimplants 4. Fabrication 4. Fabrication and Tests Tests of Recently, manufacturing and of Medical Medical Nanoimplants and successful testing of several medical implants fabricated from Nanoimplants nanostructured Ti have been Recently, manufacturingconsidered manufacturing and successful[17]. in detail and successful Another testing example of several several of the innovative medical development implants fabricated fabricated from Recently, testing of medical implants from is nanostructured the manufacturing Ti and havetesting been of the implant considered inpins designed detail [17]. for surgery Another in the example bone of tissue the of the innovative nanostructured Ti have been considered in detail [17]. Another example of the innovative hip, which increases development thebone is the strength and manufacturing andprevents testing ofitsthe of fracture implant(Figure 9) [75]. The pins designed designed pins of two for surgery surgery types in the the bone development is manufacturing and testing the implant pins for in bone tissue of the hip, which increases bone strength and prevents its fracture (Figure 9) [75]. tissue of the hip, which increases bone strength and prevents its fracture (Figure 9) [75]. The pins of The pins of
Materials 2020, 13, 967 10 of 16 Materials 2020, 13, 967 10 of 15 Materials 2020, 13, 967 10 of 15 two types (Figure 10)(Figure 10) were from were produced produced from nanostructured nanostructured Ti rods of Ti 3 mmrodsdiameter of 3 mm with diameter verywith highvery high strength two (σ types strength = 1300 (σ (Figure = 1300 MPa). 10) MPa). These were produced These were implants implants from usedwerenanostructured to studyusedtheir to study Ti rods effecttheir on theof 3 effectmm boneon diameter the bone strength with very of strength high of the the hip, which strength hip, which (σ = was1300 MPa). evaluated These by implants means of were bench used testing to study [76]. For their this was evaluated by means of bench testing [76]. For this purpose, a special device (Figure 11) was usedeffect purpose, on the a bone special strength device of the (Figure hip, to which 11)analyze was used was the to evaluated analyze the mechanical by means mechanical properties of bench testing properties of implant [76]. of implant systems For this under systems purpose, compression a underalong special device compression the axis of (Figure along the the hip. 11) axiswas Such of used the systems hip.to Such wereanalyze the mechanical systems subjected towere a defined properties subjectedload to of theimplant a defined along axis load systems along of the hip,the under as axis of well compression as the hip, in the as along well asthe perpendicular in axis the of the hip. perpendicular Such systems direction were with a subjected force to directed a defined to the load region along of the direction with a force directed to the region of the greater trochanter to complete fracture at a rate ofthe axis greater of the hip, trochanter as to well as complete in 5the perpendicular fracture mm/min atusing a ratethedirection of 5 mm INSTRON with /a force 5982 min directed using High (Instron®, to the the region of INSTRON Wycombe, the greater 5982 trochanter (Instron®, Buckinghamshire, High UK) toWycombe, complete multipurpose fracture one at a rateUK) Buckinghamshire, pin dynamometer. ofAmultipurpose 5total mm of 3/ systems min oneusing pin the INSTRON weredynamometer. studied: threeA 5982 total pins, a of (Instron®, 3 systems spiral, and a were High spiral Wycombe, studied: + pin three system. Buckinghamshire, pins, a spiral, and UK) a multipurpose spiral + pin system. one pin As a dynamometer. result [76], the A use total of of 3 systems different As a result [76], the use of different implants demonstrated high efficiency in improving the strength of were implants studied: three demonstrated pins, bone aefficiency spiral, high tissue in and the a spiral in hip. improving + pinthesystem. In particular, strength the useAsofof a bone result [76], tissue a spiral and the usehip. ina the pin of the in different implants In bone-implant particular, demonstrated thesystem use of made a spiralit high and aefficiency pin in thein improving bone-implant the strength system made of bone it tissue possible toin the increase hip.the possible to increase the axial load resistance by 72.6% in comparison to the tests excluding implants. In particular, axial load the use resistance of a by spiral 72.6% and This ademonstrated pin in the to in comparison bone-implant the prospect the system tests excluding made itofpossible implants. of integration toreinforcement increase the the This demonstrated surgical axial load prospect of the resistance hip made by 72.6% of integration of nano CP Tiof in intocomparison surgical to the reinforcement clinical practice to tests of theexcluding prevent hip implants. madebones. broken of nano CP This demonstrated Ti into clinical practicethe prospect to prevent of broken integration bones.of surgical reinforcement of the hip made of nano CP Ti into clinical practice to prevent broken bones. Figure 9. The image of the hip after the insertion of reinforcing implants. Figure Figure 9. The image 9. The image of of the the hip hip after after the the insertion insertion of of reinforcing reinforcing implants. implants. (a) (a) (b) (b) Figure 10. Figure 10. Two Twotypes typesof ofthe theimplant implantsystems systemsused: used: ((a) ((a) aa pin; pin; (b) (b) aa spiral) spiral) and and their their application application using using Figure the 10. INSTRONTwo types 5982 of the implant dynamometer. the INSTRON 5982 dynamometer. systems used: ((a) a pin; (b) a spiral) and their application using the INSTRON 5982 dynamometer.
Materials 2020, 13, 967 11 of 16 Materials 2020, 13, 967 11 of 15 Figure Figure 11. Testing Testing procedure of the reinforced hip sample. interesting example Another interesting exampleofofthe theinnovative innovativeapplication application is the is the removable removable clipping clipping device device for for blood vessels, tubular structures, and soft tissues fabricated from UFG blood vessels, tubular structures, and soft tissues fabricated from UFG NiTi with enhanced shape- NiTi with enhanced shape-memory memory effectdesigned effect and and designed for bleeding for bleeding control control duringduring laparoscopic laparoscopic operations. operations. This This device device has has been been created created andand tested tested in collaboration in collaboration between between UfaUfa State State AviationTechnical Aviation TechnicalUniversity University(USATU) (USATU) and National University of Science and Technology Technology “MISIS” “MISIS” [24]. [24]. The conducted tests demonstrated that the removable removable clipping devices produced from UFG NiTi NiTi alloy obtain several advantages when compared to the standard counterpart. Table obtain several advantages when compared to the standard counterpart. Table 2 provides the 2 provides the most important most properties important of the clipping properties device for of the clipping the UFG device andUFG for the conventional CG alloy. The and conventional CG maximum alloy. The opening angle maximum of theangle opening jaws, of at which no residual the jaws, at whichdeformation no residual was observed,was deformation increases 160◦ , which up toincreases observed, up is significantly higher than that of benchmark CG alloy. The value of the reversible to 160°, which is significantly higher than that of benchmark CG alloy. The value of the reversible shape memory effect (up shape to 4 mm) memory and(up effect the to maximum 4 mm) and ratedthe force that develops maximum rated at triggering force the clipping that develops device (upthe at triggering to 0.9 N) also clipping doubles device (up in to the 0.9 product from UFG N) also doubles alloys. in the product from UFG alloys. Table 2. Table Service characteristics 2. Service characteristics of of the the clipping clipping device device produced produced from from the the NITi NITi alloys. alloys. Material Opening Angleofof Opening Angle the Opening of the Opening Jaws of the atatReversible Jaws Reversible Max MaxRated Rated Force ofthe Force of the Material ◦ theJaws, Jaws, ° Shape Shape Memory Memory Effect,mm Effect, mm Clipping Device, Clipping Device, HН CG CG
Materials 2020, 13, 967 12 of 16 and formation of secondary phase precipitations allows for considerable improvement of the strength and fatigue properties. In the present paper the advantages of nanostructuring were demonstrated for CP Ti, Ti alloys including new β-Ti alloys as well as the NiTi alloy with shape memory effect. The approaches to computer design of a number of miniaturized medical implants made from high-strength nanomaterials have been suggested. In addition, the paper includes the examples of manufacturing and tests of selected advanced medical devices for traumatology and surgery from Ti nanobiomaterials. Taking into account the results of recent studies on surface modification, including chemical etching of nanometals and deposition of bioactive coatings, it is assumed that the developments of Ti-based nanomaterials opens new possibilities for advanced medical implants and devices with improved design and functionality. Author Contributions: R.Z.V. introduced the concept and contents of the present paper, together with co-authors conducted the analysis and description of the resulting data. E.A.P. prepared the results of studies on the structure and properties of UFG TiNi alloy with shape memory effect. N.A.K. provided the results of the design of miniaturized implants (Section 3). G.I.R. provided the description of SPD techniques for processing CP Ti and Ti alloys to produce UFG structure. T.B.M. introduced the original data on manufacturing and testing of the implant pins designed for surgery in the bone tissue of the hip. J.S. reviewed the results of studies on biomedical Ti alloys subjected to SPD processing. All authors have read and agreed to the published version of the manuscript. Funding: This research was funded by Russian Science Foundation grant № 19-49-02003 and by Ministry of Education, Youth and Sports of the Czech Republic (project №LTARF18010). The authors gratefully acknowledge the financial support from Saint Petersburg State University in the framework of Call 3 project (id 26130576 for R.Z.V., E.A.P. and N.A.K.). This work was also financially by Ministry of Industry and Trade of the Czech Republic (project № FV20147). Conflicts of Interest: The authors declare no conflict of interest. References 1. Hanawa, T. Overview of metals and applications. In Metals for Biomedical Devices; Elsevier BV: Amsterdam, The Netherlands, 2010; pp. 3–24. 2. Froes, F.H.; Qian, M. Titanium in Medical and Dental Applications, 1st ed.; Woodhead Publishing: Duxford, UK, 2018. 3. Valiev, R.; Islamgaliev, R.; Alexandrov, I. Bulk nanostructured materials from severe plastic deformation. Prog. Mater. Sci. 2000, 45, 103–189. [CrossRef] 4. Valiev, R.Z.; Estrin, Y.; Horita, Z.; Langdon, T.G.; Zehetbauer, M.J.; Zhu, Y.T. Producing bulk ultrafine-grained materials by severe plastic deformation: Ten years later. JOM 2016, 68, 1216–1226. [CrossRef] 5. Valiev, R.Z.; Estrin, Y.; Horita, Z.; Langdon, T.G.; Zehetbauer, M.J.; Zhu, Y.T. Fundamentals of superior properties in bulk nanoSPD materials. Mater. Res. Lett. 2016, 4, 1–21. [CrossRef] 6. Whang, S.H. Nanostructured Metals and Alloys: Processing, Microstructure, Mechanical Properties and Applications, 1st ed.; Woodhead Publishing Limited: Cambridge, UK, 2011. 7. Rosochowski, A. Severe Plastic Deformation Technology; Whittles Publishing: Scotland, UK, 2017. 8. Estrin, Y.; Vinogradov, A. Extreme grain refinement by severe plastic deformation: A wealth of challenging science. Acta Mater. 2013, 61, 782–817. [CrossRef] 9. Valiev, R.Z.; Langdon, T.G. Principles of equal-channel angular pressing as a processing tool for grain refinement. Prog. Mater. Sci. 2006, 51, 881–981. [CrossRef] 10. Rack, H.J.; Qazi, J.; Allard, L.; Valiev, R.Z. Thermal Stability of Severe Plastically Deformed VT-6 (Ti-6Al-4V). Mater. Sci. Forum 2008, 584, 893–898. [CrossRef] 11. Takizawa, Y.; Masuda, T.; Fujimitsu, K.; Kajita, T.; Watanabe, K.; Yumoto, M.; Otagiri, Y.; Horita, Z. Scaling up of High-Pressure Sliding (HPS) for Grain Refinement and Superplasticity. Met. Mater. Trans. A 2016, 47, 4669–4681. [CrossRef] 12. Fakhretdinova, E.I.; Raab, G.I.; Valiev, R.Z. Modeling of Metal Flow during Processing by Multi-ECAP-Conform. Adv. Eng. Mater. 2015, 17, 1723–1727. [CrossRef] 13. Valiev, R.Z. Nanostructuring of metals by severe plastic deformation for advanced properties. Nat. Mater. 2004, 3, 511–516. [CrossRef]
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