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Recent Advances in Structural Carbon Nanotube Composites

Carbon nanotubes (CNT) have been a subject of investigation for more than two decades. Part of the interest in CNTs was driven by CNT tensile mechanical properties at the nanoscale that suggest their potential to outperform state-of-the-art (SOA) lightweight structural materials. Early work on the development of CNT nanocomposites involved the dispersion of CNT powder into polymer matrices. Although low levels of CNT doping resulted in meaningful increases in electrical conductivity to enable applications such as electrostatic charge dissipation, the highest concentrations of CNTs in these lightly doped nanocomposites did not yield mechanical properties that could compete with SOA carbon fiber composites. The maximum concentration of CNTs in lightly doped nanocomposites was limited to about 5% due to increases in viscosity that prevent the fabrication of good quality nanocomposites. At the lower concentrations, properties of the resulting nanocomposites were analogous to those of composites made with very short, chopped carbon fibers. About ten years ago, CNTs became available in continuous fiber form, allowing the investigation of processing methods to incorporate much higher CNT content into composites. Recent developments in CNT composite fabrication have yielded improved mechanical properties and indicate that while some standard carbon fiber composite processing methods can be used, CNTs have unique microstructural features that require techniques tailored to access the hierarchical features of CNTs. This presentation will discuss the evolution of structural CNT mechanical property advancements and collaboration mechanisms for research across federal labs, academia, and industry that accelerated the maturation of structural CNTs.

Carbon Nanotubes↗
NASA NTRS2018

Undirectional Carbon Nanotube Yarn/Polymer Composites

Carbon nanotubes (CNTs) are one-dimensional nanomaterials with outstanding electrical and thermal conductivities and mechanical properties at the nanoscale. With these superior physical properties, CNTs are very attractive materials for future light weight structural aerospace applications. Recent manufacturing advances have led to the availability of bulk formats of CNTs such as yarns, tapes, and sheets in commercial quantities, thus enabling the development of macroscale composite processing methods for aerospace applications. The fabrication of unidirectional CNT yarn/polymer composites and the effect of processing parameters such as resin type, number of CNT yarn layers, CNT yarn/resin ratio, consolidation method, and tension applied during CNT yarn winding on the mechanical properties of unidirectional CNT yarn composites are reported herein. Structural morphologies, electrical and thermal conductivities, and mechanical performance of unidirectional CNT yarn/polymer composites under tensile and short beam shear loads are presented and discussed. The application of higher tension during the winding process and elevated cure pressure during the press molding step afforded a compact structural morphology and reduced void content in the composite. However, the composite tensile strength was negligibly impacted by the fabrication parameters, such as cure pressure, winding tension, and resin chemistry, excepting resin content and number of CNT yarn layers. The tension winding method produced better quality and lower resin content CNT yarn composites compared to conventional prepregging methods, resulting in higher specific strength and modulus of the composites. The specific tensile strength of the CNT composite was approximately 69 % of the starting CNT yarn. Electrical and thermal conductivities of unidirectional CNT yarn/polymer composites were in the range of 1000 to 12000 S/cm and 22 to 45 W/mK, respectively.

Kim, Jae-Woo↗
NASA NTRS2016

Molecular Dynamics Modeling of Carbon Nanotube Composite Fracture Using ReaxFF

Carbon nanotube (CNT) fiber reinforced composites with specific tensile strengths and moduli approaching those of aerospace grade carbon fiber composites have recently been reported. This achievement was enabled by the emerging availability of high N/tex yarns in kilometer-scale quantities. While the production of this yarn is an impressive advance, its strength is still much lower than that of the individual CNTs comprising the yarn. Closing this gap requires understanding load transfer between CNTs at the nanometer dimensional scale. This work uses reactive molecular dynamics simulations to gain an understanding at the nanometer scale of the key factors that determine CNT nanocomposite mechanical performance, and to place more realistic upper bounds on the target properties. While molecular dynamics simulations using conventional force fields can predict elastic properties, the ReaxFF reactive forcefield can also model fracture behavior because of its ability to accurately describe bond breaking and formation during a simulation. The upper and lower bounds of CNT composite properties are investigated by comparing systems composed of CNTs continuously connected across the periodic boundary with systems composed of finite length CNTs. These lengths, effectively infinite for the continuous tubes and an aspect ratio of 13 for the finite length case, result from practical limitations on the number of atoms that can be included in a simulation. Experimentally measured aspect ratios are typically on the order of 100,000, so the calculated results should represent upper and lower limits on experimental mechanical properties. Finally, the effect of various degrees of covalent crosslinking between the CNTs and amorphous carbon matrix is considered to identify the amount of CNT-matrix covalent bonding that maximizes overall composite properties.

Jensen, Benjamin D.↗
NASA NTRS2015

Effects of Atomic-Scale Structure on the Fracture Properties of Amorphous Carbon - Carbon Nanotube Composites

The fracture of carbon materials is a complex process, the understanding of which is critical to the development of next generation high performance materials. While quantum mechanical (QM) calculations are the most accurate way to model fracture, the fracture behavior of many carbon-based composite engineering materials, such as carbon nanotube (CNT) composites, is a multi-scale process that occurs on time and length scales beyond the practical limitations of QM methods. The Reax Force Field (ReaxFF) is capable of predicting mechanical properties involving strong deformation, bond breaking and bond formation in the classical molecular dynamics framework. This has been achieved by adding to the potential energy function a bond-order term that varies continuously with distance. The use of an empirical bond order potential, such as ReaxFF, enables the simulation of failure in molecular systems that are several orders of magnitude larger than would be possible in QM techniques. In this work, the fracture behavior of an amorphous carbon (AC) matrix reinforced with CNTs was modeled using molecular dynamics with the ReaxFF reactive forcefield. Care was taken to select the appropriate simulation parameters, which can be different from those required when using traditional fixed-bond force fields. The effect of CNT arrangement was investigated with three systems: a single-wall nanotube (SWNT) array, a multi-wall nanotube (MWNT) array, and a SWNT bundle system. For each arrangement, covalent bonds are added between the CNTs and AC, with crosslink fractions ranging from 0-25% of the interfacial CNT atoms. The SWNT and MWNT array systems represent ideal cases with evenly spaced CNTs; the SWNT bundle system represents a more realistic case because, in practice, van der Waals interactions lead to the agglomeration of CNTs into bundles. The simulation results will serve as guidance in setting experimental processing conditions to optimize the mechanical properties of CNT composites.

Jensen, Benjamin D.↗
NASA NTRS2016

High Volume Fraction Carbon Nanotube Composites for Aerospace Applications

Reported mechanical properties of carbon nanotubes (CNTs) at the nanoscale suggest their potential to enable significantly lighter structures of interest for space applications. However, their utility depends on the retention of these properties in bulk material formats that permit practical fabrication of large structures. This presentation summarizes recent progress made to produce carbon nanotube composites with specific tensile properties that begin to rival those of carbon fiber reinforced polymer composites. CNT content in these nanocomposites was greater than 70% by weight. Tested nanocomposite specimens were fabricated from kilometers or tens of square meters of CNT, depending on the starting material format. Processing methods to yield these results, and characterization and testing to evaluate the performance of these composites will be discussed. The final objective is the demonstration of a CNT composite overwrapped pressure vessel to be flight tested in the Fall of 2016.

Siochi, E. J.↗
NASA NTRS2015

High Volume Fraction Carbon Nanotube Composites for Aerospace Applications

Reported nanoscale mechanical properties of carbon nanotubes (CNTs) suggest that their use may enable the fabrication of significantly lighter structures for use in space applications. To be useful in the fabrication of large structures, however, their attractive nanoscale properties must be retained as they are scaled up to bulk materials and converted into practically useful forms. Advances in CNT production have significantly increased the quantities available for use in manufacturing processes, but challenges remain with the retention of nanoscale properties in larger assemblies of CNTs. This work summarizes recent progress in producing carbon nanotube composites with tensile properties approaching those of carbon fiber reinforced polymer composites. These advances were achieved in nanocomposites with CNT content of ~70% by weight. The processing methods explored to yield these CNT composite properties will be discussed, as will the characterization and test methods that were developed to provide insight into the factors that contribute to the enhanced tensile properties. Technology maturation was guided by parallel advancements in computational modeling tools that aided in the interpretation of experimental data.

Siochi, Emilie J.↗
NASA NTRS2006

Modeling of Interfacial Modification Effects on Thermal Conductivity of Carbon Nanotube Composites

The effect of functionalization of carbon nanotubes on the thermal conductivity of nanocomposites has been studied using a multi-scale modeling approach. These results predict that grafting linear hydrocarbon chains to the surface of a single wall carbon nanotube with covalent chemical bonds should result in a significant increase in the thermal conductivity of these nanocomposites. This is due to the decrease in the interfacial thermal (Kapitza) resistance between the single wall carbon nanotube and the surrounding polymer matrix upon chemical functionalization. The nanocomposites studied here consist of single wall carbon nanotubes in a bulk poly(ethylene vinyl acetate) matrix. The nanotubes are functionalized by end-grafting linear hydrocarbon chains of varying length to the surface of the nanotube. The effect which this functionalization has on the interfacial thermal resistance is studied by molecular dynamics simulation. Interfacial thermal resistance values are calculated for a range of chemical grafting densities and with several chain lengths. These results are subsequently used in an analytical model to predict the resulting effect on the bulk thermal conductivity of the nanocomposite.

Clancy, Thomas C.↗
NASA NTRS2002

Polymer-Single Wall Carbon Nanotube Composites for Potential Spacecraft Applications

Polymer-single wall carbon nanotube (SWNT) composite films were prepared and characterized as part of an effort to develop polymeric materials with improved combinations of properties for potential use on future spacecraft. Next generation spacecraft will require ultra-lightweight materials that possess specific and unique combinations of properties such as radiation and atomic oxygen resistance, low solar absorptivity, high thermal emissitivity, electrical conductivity, tear resistance, ability to be folded and seamed, and good mechanical properties. The objective of this work is to incorporate sufficient electrical conductivity into space durable polyimides to mitigate static charge build-up. The challenge is to obtain this level of conductivity (10(exp -8) S/cm) without degrading other properties of importance, particularly optical transparency. Several different approaches were attempted to fully disperse the SWNTs into the polymer matrix. These included high shear mixing, sonication, and synthesizing the polymers in the presence of pre-dispersed SWNTs. Acceptable levels of conductivity were obtained at loading levels less than one tenth weight percent SWNT without significantly sacrificing optical properties. Characterization of the nanocomposite films and the effect of SWNT concentration and dispersion on the conductivity, solar absorptivity, thermal emissivity, mechanical and thermal properties were discussed. Fibers and non-woven porous mats of SWNT reinforced polymer nanocomposite were produced using electrospinning.

Park, C.↗
NASA NTRS1999

Carbon Nanotube Composites: Strongest Engineering Material Ever?

The primary goal of the carbon nanotube project at Johnson Space Center (JSC) is to fabricate structural materials with a much higher strength-to-weight ratio than any engineered material today, Single-wall nanotubes present extraordinary mechanical properties along with new challenges for materials processing. Our project includes nanotube production, characterization, purification, and incorporation into applications studies. Now is the time to move from studying individual nanotubes to applications work. Current research at JSC focuses on structural polymeric materials to attempt to lower the weight of spacecraft necessary for interplanetary missions. These nanoscale fibers present unique new challenges to composites engineers. Preliminary studies show good nanotube dispersion and wetting by the epoxy materials. Results of tensile strength tests will also be reported. Other applications of nanotubes are also of interest for energy storage, gas storage, nanoelectronics, field emission, and biomedical uses.

Mayeaux, Brian↗
NASA NTRS2014

Processing and Characterization of Carbon Nanotube Composites

Recent advances in the synthesis of large-scale quantities of carbon nanotubes (CNT) have provided the opportunity to study the mechanical properties of polymer matrix composites using these novel materials as reinforcement. Nanocomp Technologies, Inc. currently supplies large sheets with dimensions up to 122 cm x 244 cm containing both single-wall and few-wall CNTs. The tubes are approximately 1 mm in length with diameters ranging from 8 to 12 nm. In the present study being conducted at NASA Langley Research Center (LaRC), single and multiple layers of CNT sheets were infused or coated with various polymer solutions that included commercial toughened-epoxies and bismaleimides, as well as a LaRC developed polyimide. The resulting CNT composites were tested in tension using a modified version of ASTM D882-12 to determine their strength and modulus values. The effects of solvent treatment and mechanical elongation/alignment of the CNT sheets on the tensile performance of the composite were determined. Thin composites (around 50 wt% CNT) fabricated from acetone condensed and elongated CNT sheets with either a BMI or polyimide resin solution exhibited specific tensile moduli approaching that of toughened epoxy/ IM7 carbon fiber unidirectional composites.

Can, Roberto J.↗
NASA NTRS2005

Preparation and Characterization of PETI-330/Multiwalled Carbon Nanotube Composites

As part of an ongoing effort to incorporate multi-functionality into advanced composites, blends of PETI-330 and multi-walled carbon nanotubes (MWCNTs) were prepared, characterized and fabricated into moldings. The PETI-330/MWCNT mixtures were prepared at concentrations ranging from 3 to 25 weight percent by dry mixing the components in a ball mill. The resulting powders were characterized for degree of mixing, thermal and rheological properties. Based on the characterization results, PETI-330/MWCNT samples were scaled up to approx. 300 g and used to fabricate moldings 10.2 cm x 15.2 cm x 0.32 cm thick. The moldings were fabricated by injecting the mixtures at 260-280 C into a stainless steel tool followed by curing for 1 h at 371 C. The tool was designed to impart high shear during the injection process in an attempt to achieve some alignment of the MWCNTs in the flow direction. Good quality moldings were obtained that were subsequently characterized for thermal, mechanical and electrical properties. The degree of dispersion and alignment of the MWCNTs were investigated using high-resolution scanning electron microscopy and Raman spectroscopy. The preparation and preliminary characterization of PETI-330/MWCNT composites will be discussed. Keywords: phenylethynyl terminated imides, high temperature polymers, nanocomposites,

Ghose, Sayata↗
NASA NTRS1999

Virtual Prototyping for Carbon Nanotubes and Their Compositions

Carbon nanotubes (CNT) are of interest as constituents-reinforcements for composites, probes for scanning microscopy, quantum wires for electronics, and building blocks for nanomachinery. Their small size makes direct experimental measurements difficult. Therefore, the critical answers about their properties should be obtained based on adequate modeling, virtual prototyping, using the methods of classical molecular dynamic (MD), in combination with the analytical methods and continuum mechanics.

Yakobson, Boris I.↗
NASA NTRS2017

Highly Conductive Wire: Cu Carbon Nanotube Composite Ampacity and Metallic CNT Buckypaper Conductivity

NASA is currently working on developing motors for hybrid electric propulsion applications in aviation. To make electric power more feasible in airplanes higher power to weight ratios are sought for electric motors. One facet to these efforts is to improve (increase) the conductivity and (lower) density of the magnet wire used in motors. Carbon nanotubes (CNT) and composites containing CNT are being explored as a possible way to increase wire conductivity and lower density. Presented here are measurements of the current carrying capacity (ampacity) of a composite made from CNT and copper. The ability of CNT to improve the conductivity of such composites is hindered by the presence of semiconductive CNT (s-CNT) that exist in CNT supplies naturally, and currently, unavoidably. To solve this problem, and avoid s-CNT, various preferential growth and sorting methods are being explored. A supply of sorted 95 metallic CNT (m-CNT) was acquired in the form of thick film Buckypaper (BP) as part of this work and characterized using Raman spectroscopy, resistivity, and density measurements. The ampacity (Acm2) of the Cu-5volCNT composite was 3.8 lower than the same gauge pure Cu wire similarly tested. The lower ampacity in the composite wire is believed to be due to the presence of s-CNT in the composite and the relatively low (proper) level of longitudinal cooling employed in the test method. Although Raman spectroscopy can be used to characterize CNT, a strong relation between the ratios of the primary peaks GGand the relative amounts of m-CNT and s-CNT was not observed. The average effective conductivity of the CNT in the sorted, 95 m-CNT BP was 2.5 times higher than the CNT in the similar but un-sorted BP. This is an indication that improvements in the conductivity of CNT composites can be made by the use of sorted, highly conductive m-CNT.

wire↗
NASA NTRS2016

Carbon Nanotube Composite Ampacity and Metallic CNT Buckypaper Conductivity

NASA is currently working on developing motors for hybrid electric propulsion applications in aviation. To make electric power more feasible in airplanes higher power to weight ratios are sought for electric motors. One facet to these efforts is to improve (increase) the conductivity and (lower) density of the magnet wire used in motors. Carbon nanotubes (CNT) and composites containing CNT are being explored as a possible way to increase wire conductivity and lower density. Presented here are measurements of the current carrying capacity (ampacity) of a composite made from CNT and copper. The ability of CNT to improve the conductivity of such composites is hindered by the presence of semiconductive CNT (s-CNT) that exist in CNT supplies naturally, and currently, unavoidably. To solve this problem, and avoid s-CNT, various preferential growth and sorting methods are being explored. A supply of sorted 95 metallic CNT (m-CNT) was acquired in the form of thick film Buckypaper (BP) as part of this work and characterized using Raman spectroscopy, resistivity, and density measurements. The ampacity (Acm2) of the Cu-5volCNT composite was 3.8 lower than the same gauge pure Cu wire similarly tested. The lower ampacity in the composite wire is believed to be due to the presence of s-CNT in the composite and the relatively low (proper) level of longitudinal cooling employed in the test method. Although Raman spectroscopy can be used to characterize CNT, a strong relation between the ratios of the primary peaks GGand the relative amounts of m-CNT and s-CNT was not observed. The average effective conductivity of the CNT in the sorted, 95 m-CNT BP was 2.5 times higher than the CNT in the similar but un-sorted BP. This is an indication that improvements in the conductivity of CNT composites can be made by the use of sorted, highly conductive m-CNT.

yarns↗
NASA NTRS2004

Thermal Conductivity of Carbon Nanotube Composite Films

State-of-the-art ICs for microprocessors routinely dissipate power densities on the order of 50 W/sq cm. This large power is due to the localized heating of ICs operating at high frequencies, and must be managed for future high-frequency microelectronic applications. Our approach involves finding new and efficient thermally conductive materials. Exploiting carbon nanotube (CNT) films and composites for their superior axial thermal conductance properties has the potential for such an application requiring efficient heat transfer. In this work, we present thermal contact resistance measurement results for CNT and CNT-Cu composite films. It is shown that Cu-filled CNT arrays enhance thermal conductance when compared to as-grown CNT arrays. Furthermore, the CNT-Cu composite material provides a mechanically robust alternative to current IC packaging technology.

Ngo, Quoc↗
NASA NTRS2012

NARloy-Z-Carbon Nanotube Composites

Motivation: (1) NARloy-Z (Cu-3%Ag-0.5%Zr) is the state of the art, high thermal conductivity structural alloy used for making liquid rocket engine main combustion chamber liner. It has a Thermal conductivity approx 80% of pure copper. (2) Improving the thermal conductivity of NARloy-Z will help to improve the heat transfer efficiency of combustion chamber. (3)Will also help to reduce the propulsion system mass and increase performance. It will also increases thrust to weight ratio. (4) Improving heat transfer helps to design and build better thermal management systems for nuclear propulsion and other applications. Can Carbon nanotubes (CNT) help to improve the thermal conductivity (TC)of NARloy-Z? (1)CNT's have TC of approx 20X that of copper (2) 5vol% CNT could potentially double the TC of NARloy-Z if properly aligned (3) Improvement will be less if CNT s are randomly distributed, provided there is a good thermal bond between CNT and matrix. Prior research has shown poor results (1) No TC improvement in the copper-CNT composite reported (2)Reported values are typically lower (3) Attributed to high contact thermal resistance between CNT and Cu matrix (4)Results suggest that a bonding material between CNT and copper matrix is required to lower the contact thermal resistance It is hypothesized that Zr in NARloy-Z could act as a bonding agent to lower the contact thermal resistance between CNT and matrix.

Bhat, Biliyar N.↗
NASA NTRS2005

Development of Carbon-Nanotube/Polymer Composites

A report presents a short discussion of one company's effort to develop composites of carbon nanotubes in epoxy and other polymer matrices. The focus of the discussion is on the desirability of chemically modifying carbon nanotubes to overcome their inherent chemical nonreactivity and thereby enable the formation of strong chemical bonds between nanotubes and epoxies (or other polymeric matrix materials or their monomeric precursors). The chemical modification is effected in a process in which discrete functional groups are covalently attached to the nanotube surfaces. The functionalization process was proposed by the company and demonstrated in practice for the first time during this development effort. The covalently attached functional groups are capable of reacting with the epoxy or other matrix resin to form covalent bonds. Furthermore, the company uses this process to chemically modify the nanotube surfaces, affording tunable adhesion to polymers and solubility in select solvents. Flat-sheet composites containing functionalized nanotubes demonstrate significantly improved mechanical, thermal, and electrical properties.

Reynolds, Thomas A.↗
NASA NTRS2022

Building and Breaking Carbon Composites with REACTER

Carbon-based composites have become indispensable materials in aerospace and other high-performance applications, yet obtaining a detailed, nanoscale understanding of their morphology and failure mechanisms using only experimental methods remains a difficult challenge. REACTER is a versatile computational modeling tool for atomistic molecular dynamics simulations designed to model chemical reactions at the speed and length scales of classical force fields. In this work, several recent features of REACTER were applied to the creation and subsequent mechanical testing of two classes of carbon composites: carbon nanotube (CNT) composites and carbon fiber reinforced polymers (CFRP). A network of CNTs was grown dynamically using the new ‘create atoms’ feature of REACTER. The CNT filler was embedded into a polyarylacetylene (PAA) matrix by simulated in situ polymerization to obtain the final composite model. To generate the second class of carbon composite, fully carbonized (graphitic) carbon fiber morphologies were created by the method of Desai et al. [1], but using the advanced reaction constraints framework of REACTER. Two fiber models were created, representing a circular carbon fiber core and a flat surface, and similarly infiltrated with resin to obtain the final CFRP structure. Failure mechanisms were elucidated by simulating mechanically induced bond breaking, as characterized by third order DFT-based tight-binding simulations, via a reaction constraint on the total potential energy of the involved atoms.

Polymer↗