DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: High Energy Density Shape Memory Polymers Using Strain-Induced Supramolecular Nanostructures

Journal Article · · ACS Central Science

Shape memory polymers are promising materials in many emerging applications due to their large extensibility and excellent shape recovery. However, practical application of these polymers is limited by their poor energy densities (up to ~1 MJ/m3). Here, we report an approach to achieve a high energy density, one-way shape memory polymer based on the formation of strain-induced supramolecular nanostructures. As polymer chains align during strain, strong directional dynamic bonds form, creating stable supramolecular nanostructures and trapping stretched chains in a highly elongated state. Upon heating, the dynamic bonds break, and stretched chains contract to their initial disordered state. This mechanism stores large amounts of entropic energy (as high as 19.6 MJ/m3 or 17.9 J/g), almost six times higher than the best previously reported shape memory polymers while maintaining near 100% shape recovery and fixity. The reported phenomenon of strain-induced supramolecular structures offers a new approach toward achieving high energy density shape memory polymers.

Research Organization:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); US Army Research Office (ARO); National Science Foundation (NSF)
Grant/Contract Number:
AC02-76SF00515
OSTI ID:
1870414
Journal Information:
ACS Central Science, Journal Name: ACS Central Science Journal Issue: 10 Vol. 7; ISSN 2374-7943
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

References (57)

Shape-Memory Polymers journal June 2002
Unusual Aspects of Supramolecular Networks: Plasticity to Elasticity, Ultrasoft Shape Memory, and Dynamic Mechanical Properties journal December 2015
Molecularly-Engineered, 4D-Printed Liquid Crystal Elastomer Actuators journal November 2018
4D Printing of Shape Memory Materials for Textiles: Mechanism, Mathematical Modeling, and Challenges journal March 2021
Shape-Memory Effects in Polymer Networks Containing Reversibly Associating Side-Groups journal October 2007
Autonomous, Hands-Free Shape Memory in Glassy, Liquid Crystalline Polymer Networks journal April 2012
Quantitative Predictions of Shape-Memory Effects in Polymers journal December 2016
Tough and Water-Insensitive Self-Healing Elastomer for Robust Electronic Skin journal February 2018
Freestanding 3D Mesostructures, Functional Devices, and Shape-Programmable Systems Based on Mechanically Induced Assembly with Shape Memory Polymers journal October 2018
Materials as Machines journal March 2020
A Review of Shape Memory Polymers and Composites: Mechanisms, Materials, and Applications journal September 2020
Relationship between interchain spacing of amorphous polymers and blend miscibility as determined by wide-angle X-ray scattering journal July 1991
Determining the Strengths of Hydrogen Bonds in Solid-State Ammonia and Urea: Insight from Periodic DFT Calculations journal February 2003
Structural relaxation behavior of strain hardened shape memory polymer fibers for self-healing applications journal April 2013
Body temperature triggered shape-memory polymers with high elastic energy storage capacity journal January 2016
Cold, warm, and hot programming of shape memory polymers journal March 2016
Chain Dimensions and Entanglement Spacings book January 2007
A model for the onset of entanglements of transient hydrogen-bonded intermolecular structures in oligomeric poly(propylene glycol) journal July 1988
Polylactide-based polyurethane and its shape-memory behavior journal June 2006
Effect of the degree of soft and hard segment ordering on the morphology and mechanical behavior of semicrystalline segmented polyurethanes journal April 2006
Recent advances in polymer shape memory journal October 2011
Semi-crystalline two-way shape memory elastomer journal October 2011
Direct measure of crystalline domain size, distribution, and orientation in polyethylene fibers journal August 2020
Recent advances in shape–memory polymers: Structure, mechanism, functionality, modeling and applications journal December 2012
Well-Defined Shape-Memory Networks with High Elastic Energy Capacity journal July 2015
Molecular Alignment in Polyethylene during Cold Drawing Using In-Situ SANS and Raman Spectroscopy journal April 2017
Tough, Shape-Changing Materials: Crystallized Liquid Crystal Elastomers journal May 2017
An Acrylonitrile–Butadiene–Lignin Renewable Skin with Programmable and Switchable Electrical Conductivity for Stress/Strain-Sensing Applications journal December 2017
Stretch-Induced Crystallization and Phase Transitions of Poly(dimethylsiloxane) at Low Temperatures: An in Situ Synchrotron Radiation Wide-Angle X-ray Scattering Study journal October 2018
Clustering of Entanglement Points in Highly Strained Polymer Melts journal August 2019
Healable, Reconfigurable, Reprocessable Thermoset Shape Memory Polymer with Highly Tunable Topological Rearrangement Kinetics journal June 2017
Multidirectional Triple-Shape-Memory Polymer by Tunable Cross-linking and Crystallization journal January 2020
Melt-Processable Shape-Memory Elastomers Containing Bisurea Segments journal March 2021
Sustainable Thermosetting Polyurea Vitrimers Based on a Catalyst-Free Process with Reprocessability, Permanent Shape Reconfiguration and Self-Healing Performance journal October 2019
Unique Stress Whitening and High-Toughness Double-Cross-Linked Cellulose Films journal November 2018
New Design Strategy for Reversible Plasticity Shape Memory Polymers with Deformable Glassy Aggregates journal November 2014
Multivalent Assembly of Flexible Polymer Chains into Supramolecular Nanofibers journal September 2020
Theoretical Study of Urea and Thiourea. 2. Chains and Ribbons journal February 2000
Polymer entanglements journal March 1993
Surface Fractals in Block Copolymers journal April 1994
Attempt toward 1D Cross-Linked Thermoplastic Elastomers:  Structure and Mechanical Properties of a New System journal March 2005
Two-Way Reversible Shape Memory in a Semicrystalline Network journal January 2008
Aggregation of Ureido-Pyrimidinone Supramolecular Thermoplastic Elastomers into Nanofibers: A Kinetic Analysis journal September 2011
Energy Storage Capacity of Shape-Memory Polymers journal May 2013
Programming of Temperature-Memory Onsets in a Semicrystalline Polyurethane Elastomer journal July 2014
Optically healable supramolecular polymers journal April 2011
A highly stretchable autonomous self-healing elastomer journal April 2016
Reprogrammable recovery and actuation behaviour of shape-memory polymers journal January 2019
Stimulus-responsive polymers journal January 2017
Fractal properties of polymer crystals journal February 1989
Stress whitening in crystalline propylene-ethylene block copolymers journal June 1981
Nika : software for two-dimensional data reduction journal March 2012
The crystal structure and molecular thermal motion of urea at 12, 60 and 123 K from neutron diffraction journal June 1984
Artificial Muscle Technology: Physical Principles and Naval Prospects journal July 2004
Programming a crystalline shape memory polymer network with thermo- and photo-reversible bonds toward a single-component soft robot journal January 2018
Shape and Temperature Memory of Nanocomposites with Broadened Glass Transition journal November 2007
Synchrotron small-angle x-ray scattering study of linear low-density polyethylene under uniaxial deformation journal April 2012