Abstract
The environmental issues stemming from plastic waste and the excessive use of petroleum-based chemicals are both concerning and urgent. To effectively address this problem, we need to adopt a comprehensive approach involving developing more sustainable and renewable materials. These materials should be capable of demonstrating similar or even better performance than functional polymers synthesized from petroleum-based chemicals. Our research aims to develop more sustainable materials by leveraging the intrinsic characteristics of a natural polymer, lignin, a byproduct of the biorefinery industries. We utilized the three-dimensional branching structure of lignin as a material framework. We employed an approach to coreactive melt processing of kraft lignin with aliphatic flexible chains of soft cross-linkers through the reaction of the cross-linker epoxy chain ends with lignin functional groups. Our study demonstrates that the interlocked structure formed from the coblending of kraft lignin with ultrahigh molecular weight poly(ethylene oxide) and the cross-linking of lignin chains through a solvent-free process can manipulate the macromolecular interactions and relaxation. This manipulation results in materials that exhibit a wide range of thermomechanical properties and self-healing and shape memory effects, with drastically improved stiffness in a single material. We have explored the fundamental understanding of the macromolecular chain relaxation dynamics originating from the interlocking structure formation. This investigation utilized various techniques, including thermal, mechanical, rheology, and quasi-elastic neutron scattering.
Original language | English |
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Pages (from-to) | 11877-11888 |
Number of pages | 12 |
Journal | ACS Applied Polymer Materials |
Volume | 6 |
Issue number | 19 |
DOIs | |
State | Published - Oct 11 2024 |
Funding
This work was supported by the Illinois Applied Research Institute within the Grainger College of Engineering at the University of Illinois, Urbana-Champaign. Work at ORNL\u2019s Spallation Neutron Source was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy. Oak Ridge National Laboratory is managed by UT-Battelle, LLC, for U.S. DOE under Contract no. DEAC05-00OR22725. We thank Professor Jeff Baur at the Department of Aerospace Engineering, University of Illinois at Urbana-Champaign, for the Brabender access. We also thank the Illinois Applied Research Institute Laboratory and the Materials Research Laboratory, University of Illinois at Urbana-Champaign, for the characterization facility access. This work was supported by the Illinois Applied Research Institute within the Grainger College of Engineering at the University of Illinois, Urbana\u2013Champaign. Work at ORNL\u2019s Spallation Neutron Source was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy. Oak Ridge National Laboratory is managed by UT-Battelle, LLC, for U.S. DOE under Contract no. DEAC05-00OR22725. We thank Professor Jeff Baur at the Department of Aerospace Engineering, University of Illinois at Urbana\u2013Champaign, for the Brabender access. We also thank the Illinois Applied Research Institute Laboratory and the Materials Research Laboratory, University of Illinois at Urbana\u2013Champaign, for the characterization facility access.
Keywords
- dynamic bonds
- interlocking
- lignin
- self-healing
- shape memory
- transforming materials