Drastically Enhancing Moduli of Graphene-Coated Carbon Nanotube Aerogels via Densification while Retaining Temperature-Invariant Superelasticity and Ultrahigh Efficiency.

Lightweight open-cell foams that are simultaneously superelastic, possess exceptionally high Young's moduli (Y), exhibit ultrahigh efficiency, and resist fatigue as well as creep are particularly desirable as structural frameworks. Unfortunately, many of these features are orthogonal in foams of metals, ceramics, and polymers, particularly under large temperature variations. In contrast, foams of carbon allotropes including carbon nanotubes and graphene developed over the past few years exhibit these desired properties but have low Y due to low density, ρ = 0.5-10 mg/mL. Densification of these foams enhances Y although below expectation and also dramatically degrades other properties because of drastic changes in microstructure. We have recently developed size- and shape-tunable graphene-coated single-walled carbon nanotube (SWCNT) aerogels that display superelasticity at least up to a compressive strain (ε) = 80%, fatigue and creep resistance, and ultrahigh efficiency over -100-500 °C. Unfortunately, Y of these aerogels is only ∼0.75 MPa due to low ρ ≈ 14 mg/mL, limiting their competitiveness as structural foams. We report fabrication of similar aerogels but with ρ spanning more than an order of magnitude from 16-400 mg/mL through controlled isostatic compression in the presence of a polymer coating circumventing any microstructural changes in stark contrast to other foams of carbon allotropes. The compressive stress (σ) versus ε measurements show that the densification of aerogels from ρ ≈ 16 to 400 mg/mL dramatically enhances Y from 0.9 to 400 MPa while maintaining superelasticity at least up to ε = 10% even at the highest ρ. The storage (E') and loss (E″) moduli measured in the linear regime show ultralow loss coefficient, tan δ = E″/E' ≈ 0.02, that remains constant over three decades of frequencies (0.628-628 rad/s), suggesting unusually high frequency-invariant efficiency. Furthermore, these aerogels retain exceptional fatigue resistance for 106 loading-unloading cycles to ε = 2% and creep resistance for at least 30 min under σ = 0.02 MPa with ρ = 16 mg/mL and σ = 2.5 MPa with higher ρ = 400 mg/mL. Lastly, these robust mechanical properties are stable over a broad temperature range of -100-500 °C, motivating their use as highly efficient structural components in environments with extreme temperature variations.

Application of soft lithography to metal-induced lateral crystallization of amorphous Si thin films involving self-assembly monolayers and atomic layer deposition.

Micro-contact printing of self-assembly monolayers (SAMs), i.e., octadecyl-trichlorosilane (OTS) was combined with self limiting atomic layer deposition in order to fabricate the selective deposition of nickel oxide on amorphous Si thin films. The localized nickel species facilitated metal-induced crystallization (MIC) and at later stages, metal-induced lateral crystallization (MILC) in amorphous Si thin films at the elevated temperatures ranging from 500 °C to 550 °C. The uniform coating of SAMs onto amorphous Si thin films was monitored using physical/chemical characterization, i.e., atomic force microscopy, electron microscopy, and Raman spectroscopy. The crystalline feature was found to be superior to the counterpart solid-phase crystallization. The effectiveness of SAMs appears to provide the microscale patterning in addition to the sophisticated control against nickel-species.

Thermal and electrical transport in ultralow density single-walled carbon nanotube networks.

The thermal, electrical, and thermoelectric properties of aerogels of single-walled carbon nanotubes are characterized. Their ultralow density enables the transport properties of the junctions to be distinguished from those of the nanotubes themselves. Junction thermal and electrical conductances are found to be orders of magnitude larger than those found in typical dense SWCNT networks. In particular, the average junction thermal conductance is close to the theoretical maximum for a van der Waals bonded SWCNT junction.

Graphene coating makes carbon nanotube aerogels superelastic and resistant to fatigue.

Lightweight materials that are both highly compressible and resilient under large cyclic strains can be used in a variety of applications. Carbon nanotubes offer a combination of elasticity, mechanical resilience and low density, and these properties have been exploited in nanotube-based foams and aerogels. However, all nanotube-based foams and aerogels developed so far undergo structural collapse or significant plastic deformation with a reduction in compressive strength when they are subjected to cyclic strain. Here, we show that an inelastic aerogel made of single-walled carbon nanotubes can be transformed into a superelastic material by coating it with between one and five layers of graphene nanoplates. The graphene-coated aerogel exhibits no change in mechanical properties after more than 1 × 10(6) compressive cycles, and its original shape can be recovered quickly after compression release. Moreover, the coating does not affect the structural integrity of the nanotubes or the compressibility and porosity of the nanotube network. The coating also increases Young's modulus and energy storage modulus by a factor of ∼6, and the loss modulus by a factor of ∼3. We attribute the superelasticity and complete fatigue resistance to the graphene coating strengthening the existing crosslinking points or 'nodes' in the aerogel.