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Large Tunability in the Mechanical and Thermal Properties of Carbon Nanotube-Fullerene Hierarchical Monoliths

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Large Tunability in the Mechanical and Thermal Properties of Carbon Nanotube-Fullerene Hierarchical Monoliths Nanoscale Large tunability in the mechanical and thermal properties of carbon nanotube-fullerene hierarchical monoliths Journal: Nanoscale Manuscript ID NR-COM-08-2018-006848.R3 Article Type: Communication Date Submitted by the 16-Nov-2018 Author: Complete List of Authors: Giri, Ashutosh; University of Virginia, Tomko, John; University of Virginia, Mechanical and Aerospace Engineering Gaskins, John; University of Virginia, Hopkins, Patrick; University of Virginia, Page 1 of 7 Nanoscale Large tunability in the mechanical and thermal properties of carbon nanotube-fullerene hierarchical monoliths† Ashutosh Giri,∗a John Tomko,b‡ John T. Gaskins,a and Patrick E. Hopkinsab‡a† Carbon based materials have attracted much attention as 1 building blocks in technologically relevant nanocomposites wards the design and fabrication of novel nanomaterials. Car- due to their unique chemical and physical properties. Here, bon based materials are promising candidates as building blocks we propose a new class of hierarchical carbon based nano- for “bottom-up” approaches in hierarchical material systems due truss structures consisting of fullerene joints attached with to their different allotropes and the ability to form a wide range of 2–5 carbon nanotubes as the truss forming a three-dimensional geometries. Along with the aforementioned qualities, and the network. Atomistic molecular dynamics simulations allow added advantage of scalability, these materials can potentially of- us to systematically demonstrate the ability to simulta- fer large tunability in their physical and chemical properties with 6–8 neously control the mechanical and thermal properties novel and systematic design of their microstructure. Among of these structures, elucidating their unique physical the various allotropes are carbon nanotube (CNT) structures with properties. Specifically, we perform uniaxial tensile and rolled hexagonal carbon networks that possess enhanced mechan- compressive loading to show that by controlling the length ical, electrical, and thermal properties that have been considered of the carbon nanotube trusses, the mechanical properties for various technological applications and devices such as hydro- 9 10 11 can be tuned over a large range. Furthermore, we utilize gen storage, biosensors, field emission sources, and flexible 12 the Green-Kubo method under the equilibrium molecular energy storage devices, to name a few. With regards to individ- dynamics simulations framework to show that the thermal ual CNTs, their thermal and mechanical properties stand out as conductivities of these structures can be manipulated they possess exceptionally high thermal conductivities of ∼3000 −1 −1 13–15 by varying the densities of the overall structures. This W m K or higher at room temperature with ultrahigh 16 work provides a computational framework guiding future Young’s moduli of ∼1 TPa. research on the manipulation of the fundamental physical properties in these organic-based hierarchical structures As building blocks, CNTs have been joined together to 17,18 composed of carbon nanotubes and fullerenes as building form two-dimensional junctions and three-dimensional net- 19–22 blocks. works with many of the intrinsic properties of CNTs pre- served in the hierarchical structures. Theoretical studies have The promise of material systems with precise control over their demonstrated the ability to carefully guide electrical currents microstructural morphology, and those that have “user-defined” through specified paths in these hierarchical structures, which mechanical, electrical, thermal, and mass transport properties could potentially lead to CNT-based integrated electronic cir- 23–25 has driven an extensive thrust in the scientific community to- cuits. Moreover, since CNTs are hard to combine with other materials and fracture upon compressive loading, 26 the introduc- tion of chemically active fullerene molecules covalently bonded on the side walls of single-walled (SW) CNTs have shown to in- a Department of Mechanical and Aerospace Engineering, University of Virginia, Char- 27,28 lottesville, Virginia 22904, USA crease their chemical reactivity and mechanical flexibility. In b‡ Department of Materials Science and Engineering, University of Virginia, Char- this context, it is vital that investigation towards designing and lottesville, Virginia 22904, USA understanding the fundamental properties of new types of car- a† Department of Physics, University of Virginia, Charlottesville, Virginia 22904, USA bon based materials progresses with the goal of achieving novel y Electronic Supplementary Information (ESI) available: [Details of the computa- tional setup, Green Kubo approach and the mechanical properties calculations]. See structures capable of unearthing new regimes in materials and DOI: 10.1039/b000000x/ device design. Journal Name, [year], [vol.], 1–6 | 1 Nanoscale Page 2 of 7 (a) (b) 120 30 (a) (b) 100 25 80 20 60 15 Stress (GPa) 40 Stress (GPa) 10 z y 20 5 y x 0 0 x 0 0.1 0.2 0.3 0 0.1 0.2 0.3 Engineering Strain Engineering Strain 16 140 (c) (d) (c) (d) compression 14 120 tension 12 100 10 80 8 60 d 6 Stress (GPa) 40 4 Youngs Modulus (GPa) 2 20 y 0 0 0 0.1 0.2 0.3 0.375 0 0.2 0.4 0.6 0.8 1 1.2 x Engineering Strain Density (g cm-3) y z L x Fig. 2 (a) Stress-strain curves for a pristine (6,0) SWCNT and one- dimensional CNT-fullerene chains with varying CNT lengths under uni- Fig. 1 (a) Schematic of the C80 molecule with achiral icosahedral sym- axial tension. The dashed-line shows the representative linear fit to metry. The orange atoms are bonded to the open ends of the (6,0) CNT. the elastic response of the pristine (6,0) SWCNT used to determine (b) A unit cell for CNT–fullerene structure with d=17.5 Å. (c) Schematic the Young’s modulus. Stress-strain curves for three-dimensional CNT- of the front view of a computational domain for a CNT–fullerene system fullerene structures show tunability in the Young’s modulus with varying d with the CNT length of d=17.5 Å. (b) A three-dimensional view of the under uniaxial (b) tension and (c) compression. (d) Young’s modulus as computational domain for the CNT–fullerene system. a function of density for the CNT-fullerene systems under uniaxial tensile (hollow squares) and compressive (filled circles) loadings. Three-dimensional CNT-based structures generally have ex- the C80 molecule as shown in Fig. 1a allows the open ends of the citing properties for applications involving biomedical devices, fullerene to match with the hexagonal rings at opposite sides of tough electronics, automobile industries and also offer the unique the fullerene to form a three-dimensional monolith from the unit capability of significantly higher surface areas as compared to cell constructed by covalently attaching six (6,0) CNTs at the op- 33 individual bundles of CNTs, which makes them idea for en- posite ends of the C80 (as shown in Fig. 1b). Along with the 22,29–32 hanced hydrogen storage. Therefore, in this work, we symmetry considerations, another reason for using C80 and (6,0) present a theoretical study focusing on a new class of three- CNTs for the monoliths is also due to the fact that previous stud- dimensional carbon based hierarchical nano-truss structures con- ies have demonstrated that fullerenes can be covalently attached sisting of fullerene joints attached with CNTs as the trusses. to CNTs via the [6+6] cycloaddition, which entails bond forma- We utilize atomistic simulations to demonstrate that these CNT- tions of the hexagonal face of the fullerenes and six atoms in the fullerene structures exhibit large tunability in their mechanical CNT. 27,34 We vary the lengths of the CNTs (d) to create the nano- and thermal properties with the systematic manipulation of their truss systems with a range of densities and porosities with d rang- microstructure. Under the molecular dynamics (MD) framework, ing from 7 to 28 Å. The size of the simulation domain (L × L × L) we perform uniaxial tensile and compressive loading tests to elu- depends on the type of simulation (as discussed in more detail 3 cidate their unique and tunable mechanical properties. We then below) and is typically 104×104×104 Å as shown for the case utilize the Green-Kubo (GK) approach to predict the thermal con- of the nanotruss structure with d=17.5 Å in Figs. 1c and 1d. ductivities of our structures. Our results reveal that, by con- Uniaxial tensile and compressive loadings are applied in the trolling the length of the CNT trusses, the mechanical and ther- x-direction to obtain the representative stress-strain curves. Ther- mal properties of these hierarchical monolith carbon-based nan- mal conductivities are predicted utilizing the GK approach under otrusses can both be tuned by a factor of five, thus providing the the equilibrium molecular dynamics (EMD) simulations frame- knob for “user-defined” properties in these novel material sys- work; all MD simulations are performed with the LAMMPS tems. code 35 utilizing the widely used adaptive intermolecular reac- 36 Using C80 and (6,0) CNTs, we construct the nano-truss systems tive empirical bond-order (AIREBO) potential. Additional de- as shown in Fig. 1 by covalently bonding the fullerene and the tails regarding the MD calculations used to produce deformation CNT at the hexagonal rings of the fullerene and the open ends of simulations and thermal conductivity predictions are given in the the (6,0) CNTs. The hexagonal rings in the C80 that are connected Supplementary information. to the CNT to form the nano-truss systems have been highlighted Along with our nano-truss systems, we also perform uniax- in Fig. 1a as orange atoms. The achiral icosahedral symmetry of ial tensile tests on individual CNTs and one-dimesional CNT- 2 | 1–6 Journal Name, [year], [vol.], Page 3 of 7 Nanoscale (a) ε = 0.2 (a) (b) (c) (a) ε = 0.1 ε = 0.11 ε = 0.17 ε = 0.22 (d) (e) (f) (c) ε = -0.02 (d) ε = -0.15 ε = -0.05 ε = -0.08 ε = -0.15 Fig.
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