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DOE OSTI2025

Origin of Heating-Induced Softening and Enthalpic Reinforcement in Elastomeric Nanocomposites

Molecular simulations demonstrate that the enthalpic softening of elastomeric nanocomposites upon heating can arise naturally from a Poisson’s ratio mismatch between elastomer and nanoparticle networks, providing a more parsimonious explanation for this phenomenon than the widely accepted interpretation based on glassy interparticle bridging. Despite a century of use, the mechanism of nanoparticle-driven mechanical reinforcement of elastomers is unresolved. Here, a major hypothesis attributes it to glassy interparticle bridges, supported by an observed inversion of the variation of the modulus E(T) on heating – from entropic stiffening in elastomers to enthalpic softening in nanocomposites. Here, molecular simulations reveal that elastomer enthalpic softening can instead emerge from a competition over the preferred volumes between elastomer and nanoparticulate networks. A theory for this competition accounting for softening of the bulk modulus on heating predicts the simulated E(T) inversion, suggesting that reinforcement is driven by a volume-competition mechanism unique to cocontinuous systems of soft and rigid networks.

Biopolymers↗

DOE OSTI2025

Glassy interphases reinforce elastomeric nanocomposites by enhancing percolation-driven volume expansion under strain

For nearly a century, introduction of nanoparticles to elastomers has yielded extraordinarily tough nanocomposites that are critical to technologies from actuators to tires. The mechanisms by which this reinforcement occurs have nevertheless remained a central open question in material science. One widely debated hypothesis posits that strong interactions between polymer and particles induce "glassy bridges" that cement particles into a cohesive percolating network that resists elongation. Here, molecular dynamics simulations show that glassy particle shells do not primarily provide elongational cohesion. Instead, they amplify an underlying mechanism wherein competition between filler and elastomer networks causes the elastomer's volume to increase on deformation. This induces contributions from the elastomer's bulk modulus, which is of order 1000 times larger than its Young's modulus. These findings establish a unified understanding of low-strain reinforcement in filled elastomers as emanating from volumetric competition between coexisting particulate and elastomeric networks. This reframes and unifies our understanding of low-strain reinforcement, provides a clear-cut diagnostic for the presence of glassy bridging, and offers a new design principle for tough elastomeric nanocomposites.

Computational Physics (physics.comp-ph)↗

NASA NTRS2007

Space Environment's Effects on Seal Materials

A Low Impact Docking System (LIDS) is being developed by the NASA Johnson Space Center to support future missions of the Crew Exploration Vehicle (CEV). The LIDS is androgynous, such that each system half is identical, thus any two vehicles or modules with LIDS can be coupled. Since each system half is a replica, the main interface seals must seal against each other instead of a conventional flat metal surface. These sealing surfaces are also expected to be exposed to the space environment when vehicles are not docked. The NASA Glenn Research Center (NASA GRC) is supporting this project by developing the main interface seals for the LIDS and determining the durability of candidate seal materials in the space environment. In space, the seals will be exposed to temperatures of between 50 to 50 C, vacuum, atomic oxygen, particle and ultraviolet radiation, and micrometeoroid and orbital debris (MMOD). NASA GRC is presently engaged in determining the effects of these environments on our candidate elastomers. Since silicone rubber is the only class of seal elastomer that functions across the expected temperature range, NASA GRC is focusing on three silicone elastomers: two provided by Parker Hannifin (S0-899-50 and S0-383-70) and one from Esterline Kirkhill (ELA-SA-401). Our results from compression set, elastomer to elastomer adhesion, and seal leakage tests before and after various simulated space exposures will be presented.

deGroh, Henry C., III↗

NASA NTRS2010

Reducing Seal Adhesion in Low Impact Docking Systems

Silicone elastomers, used in seals for airlocks or other sealing surfaces in space, are sticky in their as-received condition. Because of the sticking, a greater force may be needed to separate the mating surfaces. If the adhesion is sufficiently high, a sudden unpredicted movement of the spacecraft during undocking, vibration, or uneven release could pull off the seal, resulting in a damage that would have to be repaired before another docking. The damaged seal can result in significant gas leakage and possibly in a catastrophic mishap impacting the safety of the crew. It is also possible that a compromised seal could result in a delayed but sudden gas leak that could put the crew at unexpected risk. This is especially of concern for androgynous seals, which have identical mating surfaces on both sides for interchangeability and redundancy. Such seals typically have elastomer-on-elastomer sealing surfaces. To reduce sticking, one could use release agents such as powders and lubricants, but these can be easily removed and transferred to other surfaces, causing uneven sealing and contamination. Modification of the elastomer surface to make a more slippery and less sticky surface that is integral with the bulk elastomer would be more desirable.

Banks, Bruce A.↗

NASA NTRS1972

Life prediction of expulsion bladders through fatigue test and fold strain analysis

Cycle life data are presented in terms of true maximum strain for four metals, two plastics, and two elastomers. The Coffin-Manson fatigue theory was applied for metals and plastics, and cut-growth fatigue theory for elastomers. The data are based on measurements made at room and elevated temperatures. It was found that double folds give rise to far severer folding strains than do simple folds. It was also found that, except for the elastomers, all the bladder materials develop surface cracks due to double folds after only one cycle. The findings indicate that metals, which are bets for premeation resistance, are worst for fatigue resistance, and vice versa for elastomers. The intermediate plastics were found to be unsatisfactory for both permeation and fatigue resistance for missions of extended duration.

Chu, H. N.↗

DOE OSTI2024

Chain rigidity controlled aggregation ability and solid-state microstructures for efficient stretchable conjugated polymer films

Stretchable conjugated polymer films with good electrical performance under mechanical deformation are highly desirable for soft electronics. However, the mechanical and electrical properties of these films, particularly in conjugated polymer:elastomer blends, are not fully understood at molecular level. Here, this study explores the relationships among molecular structure, aggregation ability, film microstructure, and the electrical/mechanical properties of three diketopyrrolopyrrole-based conjugated polymers (P1, P2, P3) with decreasing backbone rigidity and their corresponding polymer:elastomer blends. The most flexible polymer P3 shows strong aggregation, which forms highly crystalline fibers to produce fragile neat film and produces large isolated crystallites restricting charge transport in blend film. As chain rigidity increases, the P1 and P2 polymers show weaker aggregation, and produce smaller crystallites in neat films with enhanced ductility. P1 and P2 based blend films display nanocrystallites polymer networks with dispersed elastomer domains. As a result, we achieved near-constant charge mobility before and after stretching under 50 % strain for P2-based blend films with well-controlled pathways for both charge transport and energy dissipation. This study demonstrates the critical role of backbone rigidity in regulating the properties of stretchable conjugated polymer films, paving the way for more reliable and deformable materials in soft electronics.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Impact of melt viscosity on filler dispersion in elastomeric nanocomposites

Compounding of commercial nanocomposites usually involves the addition of viscosity enhancers such as binder resins in ink jet inks, and paints. Contrary to this, plasticizers such as process oils are added to reduce the melt viscosity and ease processability of reinforced elastomers. Nanofillers such as silica and carbon black are typically added to reinforce rubber and enhance performance of automotive tire treads. Filler dispersion has traditionally been qualitatively (indirectly) assessed by measuring the properties of reinforced elastomers. While dispersion can be quantified by examining filler agglomeration through surface roughness measurements and microscopy, the size-scale dependence for these hierarchical fillers has usually been ignored. Here, we have recently devised a method to quantify nano-scale dispersion of fillers using Ultra small-angle X-ray scattering (USAXS) techniques. This method is advantageous since it directly links the controllable processing/compounding parameters such as the mixing speed, mixer geometry, residence time (or mixing duration), melt density, flow gap distance, and melt viscosity to nano-scale dispersion. While our previous studies have explored the impact of different processing parameters, this study specifically investigates the impact of melt viscosity on nano-scale filler dispersion in elastomer compounds. Commercially available polybutadienes with different Mooney viscosities were used in conjunction with different grades and amounts of process oils to modify the melt viscosity.

Carbon black↗

NASA NTRS1974

Control of elasticity in cast elastomeric shock/vibration isolators

Elasticity is determined by isolators physical dimensions and by type of elastomer used. Once elastomer is selected and cast between two concentric tubes of device, isolator elasticity will remain fixed. Isolators having same dimensions can be built to different elasticity requirements using same elastomer.

Owens, L.↗

NASA NTRS1973

Investigation into reversion of polyurethane encapsulants

The effect of high humidity (95% RH) at 60 C, 70 C, 85 C and 100 C on the solid-to-liquid reversion of polyurethane elastomers (used for potting electrical connectors and conformal coating printed circuit boards) was investigated. Hardness measurements were conducted on eleven elastomers to track reversion for a 101-day period. The primary purpose of the tests was to provide data to predict service life for the polyurethane elastomers. This was not accomplished as the hardness did not deteriorate rapidly enough at the lower test temperatures. The tests did determine that the potting and coating materials most widely used on the S-1C Program are susceptible to reversion but appear adequate for service in the S-1C environment.

Lynch, C. R.↗

NASA NTRS1982

Evaluation of shear mounted elastomeric damper

Viton-70 elastomeric shear mounted damper was built and tested on a T-55 power turbine spool in the rotor's high speed balancing rig. This application of a shear mounted elastomeric damper demonstrated for the first time, the feasibility of using elastomers as the primary rotor damping source in production turbine engine hardware. The shear damper design was selected because it was compatible with actual gas turbine engine radial space constraints, could accommodate both the radial and axial thrust loads present in gas turbine engines, and was capable of controlled axial preload. The shear damper was interchangeable with the production T-55 power turbine roller bearing support so that a direct comparison between the shear damper and the production support structure could be made. Test results show that the Viton-70 elastomer damper operated successfully and provided excellent control of both synchronous and nonsynchronous vibrations through all phases of testing up to the maximum rotor speed of 16,000 rpm. Excellent correlation between the predicted and experienced critical speeds, mode shapes and log decrements for the power turbine rotor and elastomer damper assembly was also achieved.

Zorzi, E.↗

NASA NTRS1986

Polyimide Film of Increased Tear Strength

High-temperature linear aromatic polyimide with improved resistance to tearing made by new process that incorporates elastomer into polyimide. Linear aromatic condensation polyimides are materials of prime choice for use as films and coatings on advanced spacecraft and aircraft where durability at temperatures in range of 200 to 300 degree C required. Elastomer-containing polyimide film with improved toughness proves useful for applications where resistance to tearing and long-term thermal stability necessary. Desired resistance to tearing achieved by careful control of amount and chemical composition of added elastomer.

St. Clair, A. K.↗

NASA NTRS1988

Factors affecting the sticking of insects on modified aircraft wings

Previous work showed that the total number of insects sticking to an aluminum surface was reduced by coating the aluminum surface with elastomers. Due to a large number of possible experimental errors, no correlation between the modulus of elasticity, the elastomer, and the total number of insects sticking to a given elastomer was obtained. One of the errors assumed to be introduced during the road test is a variable insect flux so the number of insects striking one surface might be different from that striking another sample. To eliminate this source of error, the road test used to collect insects was simulated in a laboratory by development of an insect impacting technique using a pipe and high pressure compressed air. The insects are accelerated by a compressed air gun to high velocities and are then impacted with a stationary target on which the sample is mounted. The velocity of an object exiting from the pipe was determined and further improvement of the technique was achieved to obtain a uniform air velocity distribution.

Yi, O.↗

NASA NTRS1987

Elastomeric binders for Li-SOCl2 cell carbon electrodes

Nonoptimized elastomer bonded carbon electrodes made with 100-percent compressed Gulf Acetylene Black have demonstrated performance comparable to that of optimized Teflon bonded carbon electrodes, made from the same carbon, when tested at 1-10 mA/sq cm, at 24 and -26 C. The enhanced performance of elastomer bonded carbon electrodes appears to be due to the more uniform utilization of the carbon electrode to store insoluble discharge products, as compared to Teflon bonded carbon electrodes. With even minimal optimization of elastomer bonded carbon electrodes, significant improvement in Li-SOCl2 cell performance can be expected.

Carter, B. J.↗

NASA NTRS1989

Making Reliable Large-Diameter O-Rings

Vacuum curing yields joint-free, voidless elastomer seals. Method for manufacturing large-diameter O-rings produces them in single pieces, without bonded joints. Reduces probability trapped gases form flaws. O-rings produced, having diameters as much as 144 in. (3.66m), reliable and of high quality. Nesting upper and lower halves of mold hold elastomer rings for curing. Oil flowing through upper and lower cavities heats elastomer to cure it.

Larsen, Glade L.↗

NASA NTRS2002

Studies on Stress-Strain Relationships of Polymeric Materials Used in Space Applications

A two-year research plan was undertaken in association with Polymers Branch, NASA Glenn Research Center, to carry out experimental and modeling work relating stress and strain behavior of polymeric materials, especially elastomers and vulcanized rubber. An experimental system based on MTS (Mechanical Testing and Simulation) A/T-4 test facility environment has been developed for a broader range of polymeric materials in addition to a design of laser compatible temperature control chamber for online measurements of various strains. Necessary material processing has been accomplished including rubber compounding and thermoplastic elastomer processing via injection molding. A broad suite of testing methodologies has been identified to reveal the complex non-linear mechanical behaviors of rubbery materials when subjected to complex modes of deformation. This suite of tests required the conceptualization, design and development of new specimen geometries, test fixtures, and test systems including development of a new laser based technique to measure large multi-axial deformations. Test data has been generated for some of these new fixtures and has revealed some complex coupling effects generated during multi-axial deformations. In addition, fundamental research has been conducted concerning the foundation principles of rubber thermodynamics and resulting theories of rubber elasticity. Studies have been completed on morphological properties of several thermoplastic elastomers. Finally, a series of steps have been identified to further advance the goals of NASA's ongoing effort.

Jana, Sadhan C.↗

NASA NTRS2004

Polymeric blends for sensor and actuation dual functionality

The invention described herein supplies a new class of electroactive polymeric blend materials which offer both sensing and actuation dual functionality. The blend comprises two components, one component having a sensing capability and the other component having an actuating capability. These components should be co-processable and coexisting in a phase separated blend system. Specifically, the materials are blends of a sensing component selected from the group consisting of ferroelectric, piezoelectric, pyroelectric and photoelectric polymers and an actuating component that responds to an electric field in terms of dimensional change. Said actuating component includes, but is not limited to, electrostrictive graft elastomers, dielectric electroactive elastomers, liquid crystal electroactive elastomers and field responsive polymeric gels. The sensor functionality and actuation functionality are designed by tailoring the relative fraction of the two components. The temperature dependence of the piezoelectric response and the mechanical toughness of the dual functional blends are also tailored by the composition adjustment.

St. Clair, Terry L.↗

NASA NTRS2010

Space Environment Effects on Silicone Seal Materials

A docking system is being developed by the NASA to support future space missions. It is expected to use redundant elastomer seals to help contain cabin air during dockings between two spacecraft. The sealing surfaces are exposed to the space environment when vehicles are not docked. In space, the seals will be exposed to temperatures between 125 to -75 C, vacuum, atomic oxygen, particle and ultraviolet radiation, and micrometeoroid and orbital debris (MMOD). Silicone rubber is the only class of space flight-qualified elastomeric seal material that functions across the expected temperature range. NASA Glenn has tested three silicone elastomers for such seal applications: two provided by Parker (S0899-50 and S0383-70) and one from Esterline (ELA-SA-401). The effects of atomic oxygen (AO), UV and electron particle radiation, and vacuum on the properties of these three elastomers were examined. Critical seal properties such as leakage, adhesion, and compression set were measured before and after simulated space exposures. The S0899-50 silicone was determined to be inadequate for extended space seal applications due to high adhesion and intolerance to UV, but both S0383-70 and ELA-SA-401 seals were adequate.

deGroh, Henry C., III↗

NASA NTRS2010

An Experimental Investigation of Silicone-to-Metal Bond Strength in Composite Space Docking System Seals

The National Aeronautics and Space Administration (NASA) is currently developing a new universal docking mechanism for future space exploration missions called the Low Impact Docking System (LIDS). A candidate LIDS main interface seal design is a composite assembly of silicone elastomer seals vacuum molded into grooves in an electroless nickel plated aluminum retainer. The strength of the silicone-tometal bond is a critical consideration for the new system, especially due to the presence of small areas of disbond created during the molding process. In the work presented herein, seal-to-retainer bonds of subscale seal specimens with different sizes of intentional disbond were destructively tensile tested. Nominal specimens without intentional disbonds were also tested. Tension was applied either uniformly on the entire seal circumference or locally in one short circumferential length. Bond failure due to uniform tension produced a wide scatter of observable failure modes and measured load-displacement behaviors. Although the preferable failure mode for the seal-to-retainer bond is cohesive failure of the elastomer material, the dominant observed failure mode under the uniform loading condition was found to be the less desirable adhesive failure of the bond in question. The uniform tension case results did not show a correlation between disbond size and bond strength. Localized tension was found to produce failure either as immediate tearing of the elastomer material outside the bond region or as complete peel-out of the seal in one piece. The obtained results represent a valuable benchmark for comparison in the future between adhesion loads under various separation conditions and composite seal bond strength.

Gaier, James R.↗