Your browser doesn't support javascript.
Mostrar: 20 | 50 | 100
Resultados 1 - 20 de 66
Filtrar
Mais filtros










Intervalo de ano de publicação
1.
Small ; 15(31): e1900573, 2019 08.
Artigo em Inglês | MEDLINE | ID: mdl-31131997

RESUMO

Many natural materials present an ideal "recipe" for the development of future damage-tolerant lightweight structural materials. One notable example is the brick-and-mortar structure of nacre, found in mollusk shells, which produces high-toughness, bioinspired ceramics using polymeric mortars as a compliant phase. Theoretical modeling has predicted that use of metallic mortars could lead to even higher damage-tolerance in these materials, although it is difficult to melt-infiltrate metals into ceramic scaffolds as they cannot readily wet ceramics. To avoid this problem, an alternative ("bottom-up") approach to synthesize "nacre-like" ceramics containing a small fraction of nickel mortar is developed. These materials are fabricated using nickel-coated alumina platelets that are aligned using slip-casting and rapidly sintered using spark-plasma sintering. Dewetting of the nickel mortar during sintering is prevented by using NiO-coated as well as Ni-coated platelets. As a result, a "nacre-like" alumina ceramic displaying a resistance-curve toughness up to ≈16 MPa m½ with a flexural strength of ≈300 MPa is produced.

2.
J Mater Sci Mater Med ; 30(1): 6, 2018 Dec 29.
Artigo em Inglês | MEDLINE | ID: mdl-30594987

RESUMO

Bone substitute fabrication is of interest to meet the worldwide incidence of bone disorders. Physical chitosan hydrogels with intertwined apatite particles were chosen to meet the bio-physical and mechanical properties required by a potential bone substitute. A set up for 3-D printing by robocasting was found adequate to fabricate scaffolds. Inks consisted of suspensions of calcium phosphate particles in chitosan acidic aqueous solution. The inks are shear-thinning and consist of a suspension of dispersed platelet aggregates of dicalcium phosphate dihydrate in a continuous chitosan phase. The rheological properties of the inks were studied, including their shear-thinning characteristics and yield stress. Scaffolds were printed in basic water/ethanol baths to induce transformation of chitosan-calcium phosphates suspension into physical hydrogel of chitosan mineralized with apatite. Scaffolds consisted of a chitosan polymeric matrix intertwined with poorly crystalline apatite particles. Results indicate that ink rheological properties could be tuned by controlling ink composition: in particular, more printable inks are obtained with higher chitosan concentration (0.19 mol·L-1).


Assuntos
Fosfatos de Cálcio/química , Quitosana/química , Impressão Tridimensional , Tecidos Suporte/química , Materiais Biocompatíveis , Reologia
3.
ACS Nano ; 12(12): 12638-12645, 2018 12 26.
Artigo em Inglês | MEDLINE | ID: mdl-30462484

RESUMO

Graphene-based fibers synthesized under ambient temperature have not achieved excellent mechanical properties of high toughness or tensile strength compared with those synthesized by hydrothermal strategy or graphitization and annealing treatment. Inspired by the relationship between organic/inorganic hierarchical structure, interfacial interactions, and moderate growth temperature of natural nacre, we fabricate an ultratough graphene fiber via sequential toughening of hydrogen and ionic bonding through a wet-spinning method under ambient temperature. A slight amount of chitosan is introduced to form hydrogen bonding with graphene oxide nanosheets, and the ionic bonding is formed between graphene oxide nanosheets and divalent calcium ions. The optimized sequential toughening of hydrogen and ionic bonding results in an ultratough graphene fiber with toughness of 26.3 MJ/m3 and ultimate tensile strength of 743.6 MPa. Meanwhile, the electrical conductivity of the resultant graphene fiber is as high as 179.0 S/cm. This kind of multifunctional graphene fiber shows promising applications in photovoltaic wires, flexible supercapacitor electrodes, wearable electronic textiles, fiber motors, etc. Furthermore, the strategy of sequential toughening of hydrogen and ionic bonding interactions also offers an avenue for constructing high-performance graphene-based fibers in the near future.


Assuntos
Cálcio/química , Grafite/química , Hidrogênio/química , Eletrodos , Íons/química , Estrutura Molecular , Tamanho da Partícula , Propriedades de Superfície , Temperatura
4.
ACS Nano ; 12(9): 8901-8908, 2018 09 25.
Artigo em Inglês | MEDLINE | ID: mdl-30021062

RESUMO

Natural nacre exhibits extraordinary functional and structural diversity, combining high strength and toughness. The mechanical properties of nacre are attributed to (i) a highly arranged hierarchical layered structure of inorganic minerals (95 vol %) containing a small amount only of organic materials (5 vol %), (ii) abundant synergistic interfacial interactions, and (iii) formation under ambient temperature. Herein, inspired by these three design principles originating from natural nacre, the supertough bioinspired graphene-based nanocomposite fibers (BGNFs) are prepared under room temperature via sequential interfacial interactions of ionic bonding and π-π interactions. The resultant synergistic effect leads to a super toughness of 18.7 MJ m-3 as well as a high tensile strength of 740.1 MPa. In addition, the electrical conductivity of these supertough BGNFs is as high as 384.3 S cm-1. They can retain almost 80% of this conductivity even after 1000 cycles of loading-unloading testing, which makes these BGNFs promising candidates for application in flexible and stable electrical devices, such as strain sensors and actuators.

5.
Sci Rep ; 7(1): 13759, 2017 10 23.
Artigo em Inglês | MEDLINE | ID: mdl-29062036

RESUMO

Natural structural materials like bone and shell have complex, hierarchical architectures designed to control crack propagation and fracture. In modern composites there is a critical trade-off between strength and toughness. Natural structures provide blueprints to overcome this, however this approach introduces another trade-off between fine structural manipulation and manufacturing complex shapes in practical sizes and times. Here we show that robocasting can be used to build ceramic-based composite parts with a range of geometries, possessing microstructures unattainable by other production technologies. This is achieved by manipulating the rheology of ceramic pastes and the shear forces they experience during printing. To demonstrate the versatility of the approach we have fabricated highly mineralized composites with microscopic Bouligand structures that guide crack propagation and twisting in three dimensions, which we have followed using an original in-situ crack opening technique. In this way we can retain strength while enhancing toughness by using strategies taken from crustacean shells.

6.
ACS Appl Mater Interfaces ; 9(42): 37136-37145, 2017 Oct 25.
Artigo em Inglês | MEDLINE | ID: mdl-28920439

RESUMO

The current lifestyles, increasing population, and limited resources result in energy research being at the forefront of worldwide grand challenges, increasing the demand for sustainable and more efficient energy devices. In this context, additive manufacturing brings the possibility of making electrodes and electrical energy storage devices in any desired three-dimensional (3D) shape and dimensions, while preserving the multifunctional properties of the active materials in terms of surface area and conductivity. This paves the way to optimized and more efficient designs for energy devices. Here, we describe how three-dimensional (3D) printing will allow the fabrication of bespoke devices, with complex geometries, tailored to fit specific requirements and applications, by designing water-based thermoresponsive inks to 3D-print different materials in one step, for example, printing the active material precursor (reduced chemically modified graphene (rCMG)) and the current collector (copper) for supercapacitors or anodes for lithium-ion batteries. The formulation of thermoresponsive inks using Pluronic F127 provides an aqueous-based, robust, flexible, and easily upscalable approach. The devices are designed to provide low resistance interface, enhanced electrical properties, mechanical performance, packing of rCMG, and low active material density while facilitating the postprocessing of the multicomponent 3D-printed structures. The electrode materials are selected to match postprocessing conditions. The reduction of the active material (rCMG) and sintering of the current collector (Cu) take place simultaneously. The electrochemical performance of the rCMG-based self-standing binder-free electrode and the two materials coupled rCMG/Cu printed electrode prove the potential of multimaterial printing in energy applications.

7.
ACS Appl Mater Interfaces ; 9(38): 32977-32989, 2017 Sep 27.
Artigo em Inglês | MEDLINE | ID: mdl-28898053

RESUMO

Many 3D printing technologies are based on the development of inks and pastes to build objects through droplet or filament deposition (the latter also known as continuous extrusion, robocasting, or direct ink writing). Controlling and tuning rheological behavior is key for successful manufacturing using these techniques. Different formulations have been proposed, but the search continues for approaches that are clean, flexible, robust and that can be adapted to a wide range of materials. Here, we show how graphene oxide (GO) enables the formulation of water-based pastes to print a wide variety of materials (polymers, ceramics, and steel) using robocasting. This work combines flow and oscillatory rheology to provide further insights into the rheological behavior of suspensions combining GO with other materials. Graphene oxide can be used to manipulate the viscoelastic response, enabling the formulation of pastes with excellent printing behavior that combine shear thinning flow and a fast recovery of their elastic properties. These inks do not contain other additives, only GO and the material of interest. As a proof of concept, we demonstrate the 3D printing of additive-free graphene oxide structures as well as polymers, ceramics, and steel. Due to its amphiphilic nature and 2D structure, graphene oxide plays multiple roles, behaving as a dispersant, viscosifier, and binder. It stabilizes suspensions of different powders, modifies the flow and viscoelasticity of materials with different chemistries, particle sizes and shapes, and binds the particles together, providing green strength for manual handling. This approach enables printing complex 3D ceramic structures using robocasting with similar properties to alternative formulations, thus demonstrating the potential of using 2D colloids in materials manufacturing.

8.
ACS Appl Mater Interfaces ; 9(29): 24987-24992, 2017 Jul 26.
Artigo em Inglês | MEDLINE | ID: mdl-28682591

RESUMO

Graphene composite films inspired by nacre are the subject of ongoing research efforts to optimize their properties for applications in flexible energy devices. Noncovalent interactions do not cause interruption of the delocalized conjugated π-electron system, thus preserving graphene's excellent properties. Herein, we synthesized a conjugated molecule with pyrene groups on both ends of a long linear chain (AP-DSS) from 1-aminopyrene (AP) and disuccinimidyl suberate (DSS). The AP-DSS molecules are used to cross-link adjacent graphene nanosheets via π-π interfacial interactions to improve properties of graphene films. The tensile strength and toughness of resultant graphene films were 4.1 and 6.4 times higher, respectively, than that of pure rGO film. More remarkably, the electrical conductivity showed a simultaneous improvement, which is rare to be achieved in other kinds of covalent or noncovalent functionalization. Such integration demonstrates the advantage of this work to previously reported noncovalent functionalization of graphene.

9.
Nat Commun ; 8: 14425, 2017 02 09.
Artigo em Inglês | MEDLINE | ID: mdl-28181518

RESUMO

The properties of graphene open new opportunities for the fabrication of composites exhibiting unique structural and functional capabilities. However, to achieve this goal we should build materials with carefully designed architectures. Here, we describe the fabrication of ceramic-graphene composites by combining graphene foams with pre-ceramic polymers and spark plasma sintering. The result is a material containing an interconnected, microscopic network of very thin (20-30 nm), electrically conductive, carbon interfaces. This network generates electrical conductivities up to two orders of magnitude higher than those of other ceramics with similar graphene or carbon nanotube contents and can be used to monitor 'in situ' structural integrity. In addition, it directs crack propagation, promoting stable crack growth and increasing the fracture resistance by an order of magnitude. These results demonstrate that the rational integration of nanomaterials could be a fruitful path towards building composites combining unique mechanical and functional performances.

10.
Sci Rep ; 6: 25059, 2016 05 05.
Artigo em Inglês | MEDLINE | ID: mdl-27146382

RESUMO

Strong and tough natural composites such as bone, silk or nacre are often built from stiff blocks bound together using thin interfacial soft layers that can also provide sacrificial bonds for self-repair. Here we show that it is possible exploit this design in order to create self-healing structural composites by using thin supramolecular polymer interfaces between ceramic blocks. We have built model brick-and-mortar structures with ceramic contents above 95 vol% that exhibit strengths of the order of MPa (three orders of magnitude higher than the interfacial polymer) and fracture energies that are two orders of magnitude higher than those of the glass bricks. More importantly, these properties can be fully recovered after fracture without using external stimuli or delivering healing agents. This approach demonstrates a very promising route towards the design of strong, ideal self-healing materials able to self-repair repeatedly without degradation or external stimuli.

11.
ACS Nano ; 10(2): 1871-6, 2016 Feb 23.
Artigo em Inglês | MEDLINE | ID: mdl-26580985

RESUMO

Ultralight and strong three-dimensional (3D) silicon carbide (SiC) structures have been generated by the carbothermal reduction of SiO with a graphene foam (GF). The resulting SiC foams have an average height of 2 mm and density ranging between 9 and 17 mg cm(-3). They are the lightest reported SiC structures. They consist of hollow struts made from ultrathin SiC flakes and long 1D SiC nanowires growing from the trusses, edges, and defect sites between layers. AFM results revealed an average flake thickness of 2-3 nm and lateral size of 2 µm. In-situ compression tests in the scanning electron microscope (SEM) show that, compared with most of the existing lightweight foams, the present 3D SiC exhibited superior compression strengths and significant recovery after compression strains of about 70%.

12.
Sci Rep ; 5: 13712, 2015 Sep 08.
Artigo em Inglês | MEDLINE | ID: mdl-26348898

RESUMO

Ultra-light porous networks based on nano-carbon materials (such as graphene or carbon nanotubes) have attracted increasing interest owing to their applications in wide fields from bioengineering to electrochemical devices. However, it is often difficult to translate the properties of nanomaterials to bulk three-dimensional networks with a control of their mechanical properties. In this work, we constructed elastomeric graphene porous networks with well-defined structures by freeze casting and thermal reduction, and investigated systematically the effect of key microstructural features. The porous networks made of large reduced graphene oxide flakes (>20 µm) are superelastic and exhibit high energy absorption, showing much enhanced mechanical properties than those with small flakes (<2 µm). A better restoration of the graphitic nature also has a considerable effect. In comparison, microstructural differences, such as the foam architecture or the cell size have smaller or negligible effect on the mechanical response. The recoverability and energy adsorption depend on density with the latter exhibiting a minimum due to the interplay between wall fracture and friction during deformation. These findings suggest that an improvement in the mechanical properties of porous graphene networks significantly depend on the engineering of the graphene flake that controls the property of the cell walls.

13.
Adv Mater ; 27(32): 4788-94, 2015 Aug 26.
Artigo em Inglês | MEDLINE | ID: mdl-26178801

RESUMO

A self-healing composite is fabricated by confining a supramolecular polymer in a graphene network. The network provides electrical conductivity. Upon damage, the polymer is released and flows to reform the material. Healing is repeatable and autonomous. The composite is sensitive to pressure and flexion and recovers its mechanical and electrical properties even when rejoining cut surfaces after long exposure times.

14.
J Biomed Mater Res A ; 103(11): 3493-502, 2015 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-25940865

RESUMO

Arthritis, bone fracture, bone tumors and other musculoskeletal diseases affect millions of people across the world. Nowadays, inert and bioactive ceramics are used as bone substitutes or for bone regeneration. Their bioactivity is very much dictated by the way proteins adsorb on their surface. In this work, we compared the adsorption of albumin and fibrinogen on inert and calcium phosphates ceramics (CaPs) using attenuated total reflection Fourier transform infrared spectroscopy (ATR-FTIR) to follow in situ protein adsorption on these materials. To this effect, we developed a sol-gel technique to control the surface chemistry of an ATR-FTIR detector. Hydroxyapatite adsorbed more albumin and ß-tricalcium phosphate adsorbed more fibrinogen. Biphasic calcium phosphate presented the lowest adsorption among CaP for both proteins, illustrating the effect of surface heterogeneities. Inert ceramics adsorbed a lower amount of both proteins compared with bioactive ceramics. A significant change was observed in the conformation of the adsorbed protein versus the surface chemistry. Hydroxyapatite produced a larger loss of α-helix structure on albumin and biphasic calcium phosphate reduced ß-sheet percentage on fibrinogen. Inert ceramics produced large α-helix loss on albumin and presented weak interaction with fibrinogen. Zirconia did not adsorb albumin and titanium dioxide promoted huge denaturalization of fibrinogen.


Assuntos
Albuminas/metabolismo , Fosfatos de Cálcio/farmacologia , Cerâmica/farmacologia , Fibrinogênio/metabolismo , Adsorção , Amidas/química , Animais , Bovinos , Durapatita/farmacologia , Humanos , Espectroscopia de Infravermelho com Transformada de Fourier , Titânio/farmacologia , Difração de Raios X , Zircônio/farmacologia
15.
Adv Mater ; 27(10): 1688-93, 2015 Mar 11.
Artigo em Inglês | MEDLINE | ID: mdl-25605024

RESUMO

Responsive graphene oxide sheets form non-covalent networks with optimum rheological properties for 3D printing. These networks have shear thinning behavior and sufficiently high elastic shear modulus (G') to build self-supporting 3D structures by direct write assembly. Drying and thermal reduction leads to ultra-light graphene-only structures with restored conductivity and elastomeric behavior.

16.
Nat Mater ; 14(1): 23-36, 2015 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-25344782

RESUMO

Natural structural materials are built at ambient temperature from a fairly limited selection of components. They usually comprise hard and soft phases arranged in complex hierarchical architectures, with characteristic dimensions spanning from the nanoscale to the macroscale. The resulting materials are lightweight and often display unique combinations of strength and toughness, but have proven difficult to mimic synthetically. Here, we review the common design motifs of a range of natural structural materials, and discuss the difficulties associated with the design and fabrication of synthetic structures that mimic the structural and mechanical characteristics of their natural counterparts.


Assuntos
Materiais Biomiméticos
17.
J Bone Miner Res ; 30(5): 786-95, 2015 May.
Artigo em Inglês | MEDLINE | ID: mdl-25418329

RESUMO

Bone is a strong and tough material composed of apatite mineral, organic matter, and water. Changes in composition and organization of these building blocks affect bone's mechanical integrity. Skeletal disorders often affect bone's mineral phase, either by variations in the collagen or directly altering mineralization. The aim of the current study was to explore the differences in the mineral of brittle and ductile cortical bone at the mineral (nm) and tissue (µm) levels using two mouse phenotypes. Osteogenesis imperfecta model, oim(-/-) , mice have a defect in the collagen, which leads to brittle bone; PHOSPHO1 mutants, Phospho1(-/-) , have ductile bone resulting from altered mineralization. Oim(-/-) and Phospho1(-/-) were compared with their respective wild-type controls. Femora were defatted and ground to powder to measure average mineral crystal size using X-ray diffraction (XRD) and to monitor the bulk mineral to matrix ratio via thermogravimetric analysis (TGA). XRD scans were run after TGA for phase identification to assess the fractions of hydroxyapatite and ß-tricalcium phosphate. Tibiae were embedded to measure elastic properties with nanoindentation and the extent of mineralization with backscattered electron microscopy (BSE SEM). Results revealed that although both pathology models had extremely different whole-bone mechanics, they both had smaller apatite crystals, lower bulk mineral to matrix ratio, and showed more thermal conversion to ß-tricalcium phosphate than their wild types, indicating deviations from stoichiometric hydroxyapatite in the original mineral. In contrast, the degree of mineralization of bone matrix was different for each strain: brittle oim(-/-) were hypermineralized, whereas ductile Phospho1(-/-) were hypomineralized. Despite differences in the mineralization, nanoscale alterations in the mineral were associated with reduced tissue elastic moduli in both pathologies. Results indicated that alterations from normal crystal size, composition, and structure are correlated with reduced mechanical integrity of bone.


Assuntos
Minerais/metabolismo , Tíbia/fisiologia , Animais , Fenômenos Biomecânicos/efeitos dos fármacos , Matriz Óssea/efeitos dos fármacos , Matriz Óssea/metabolismo , Calcificação Fisiológica/efeitos dos fármacos , Fosfatos de Cálcio/farmacologia , Cristalização , Elasticidade/efeitos dos fármacos , Camundongos , Pós , Termogravimetria , Tíbia/efeitos dos fármacos , Difração de Raios X
18.
Nat Commun ; 5: 4328, 2014 Jul 07.
Artigo em Inglês | MEDLINE | ID: mdl-24999766

RESUMO

The widespread technological introduction of graphene beyond electronics rests on our ability to assemble this two-dimensional building block into three-dimensional structures for practical devices. To achieve this goal we need fabrication approaches that are able to provide an accurate control of chemistry and architecture from nano to macroscopic levels. Here, we describe a versatile technique to build ultralight (density ≥1 mg cm(-3)) cellular networks based on the use of soft templates and the controlled segregation of chemically modified graphene to liquid interfaces. These novel structures can be tuned for excellent conductivity; versatile mechanical response (elastic-brittle to elastomeric, reversible deformation, high energy absorption) and organic absorption capabilities (above 600 g per gram of material). The approach can be used to uncover the basic principles that will guide the design of practical devices that by combining unique mechanical and functional performance will generate new technological opportunities.

19.
Int J Oral Maxillofac Implants ; 28(6): e535-46, 2013.
Artigo em Inglês | MEDLINE | ID: mdl-24278949

RESUMO

With the advent of nanotechnology, an opportunity exists for the engineering of new dental implant materials. Metallic dental implants have been successfully used for decades, but they have shortcomings related to osseointegration and mechanical properties that do not match those of bone. Absent the development of an entirely new class of materials, faster osseointegration of currently available dental implants can be accomplished by various surface modifications. To date, there is no consensus regarding the preferred method(s) of implant surface modification, and further development will be required before the ideal implant surface can be created, let alone become available for clinical use. Current approaches can generally be categorized into three areas: ceramic coatings, surface functionalization, and patterning on the micro- to nanoscale. The distinctions among these are imprecise, as some or all of these approaches can be combined to improve in vivo implant performance. These surface improvements have resulted in durable implants with a high percentage of success and long-term function. Nanotechnology has provided another set of opportunities for the manipulation of implant surfaces in its capacity to mimic the surface topography formed by extracellular matrix components of natural tissue. The possibilities introduced by nanotechnology now permit the tailoring of implant chemistry and structure with an unprecedented degree of control. For the first time, tools are available that can be used to manipulate the physicochemical environment and monitor key cellular events at the molecular level. These new tools and capabilities will result in faster bone formation, reduced healing time, and rapid recovery to function.


Assuntos
Implantes Dentários , Materiais Dentários , Nanotecnologia/métodos , Osseointegração , Cerâmica , Fenômenos Químicos , Materiais Revestidos Biocompatíveis , Implantes Dentários/tendências , Materiais Dentários/química , Propriedades de Superfície
20.
Angew Chem Int Ed Engl ; 52(30): 7805-8, 2013 Jul 22.
Artigo em Inglês | MEDLINE | ID: mdl-23780923

RESUMO

Particle get-together: Surface functionalization with a branched copolymer surfactant is used to create responsive inorganic particles that can self-assemble in complex structures. The assembly process is triggered by a pH switch that reversibly activates multiple hydrogen bonds between ceramic particles (see picture; yellow) and soft templates (n-decane; green).


Assuntos
Óxido de Alumínio/química , Polímeros/química , Tensoativos/química , Ligação de Hidrogênio , Microscopia Eletrônica de Varredura , Tamanho da Partícula , Propriedades de Superfície
SELEÇÃO DE REFERÊNCIAS
DETALHE DA PESQUISA