Abstract
Polymer networks featuring dynamic bonds offer a promising solution to address key
challenges in polymer materials, especially in terms of sustainability. The dynamic
covalent chemistries enhance processability, enable recycling of the reversibly cross-
linked thermosets and elastomers, and offer repairability. Over the last 10 years, the
maturity of these networks has exponentially increased. However, they still haven’t
made it into the mass consumer market.
To stand a chance in the competitive polymer industry, dynamic polymer networks
need to further exploit their advantageous properties and enhanced performance in
combination with a focus on sustainability. This overarching objective has been divided
in three stages, where the results of each stage were sequentially added to the next
one.
The first main focus is sustainability in all its aspects. Dynamic covalent polymer
networks with self-healing properties were developed using the 12 principles of green
chemistry as the designing driving force. The sustainability was tackled from a holistic
point of view, taking into account the whole life cycle of the material (circular economy).
The developed self-healing elastomers account for the sustainability of (1) the raw
materials and (2) solvents, (3) the reusability, (4) the (re)processability, and (5) the end
of life of the material. They are synthesized by a simple one-pot, solventless synthesis
from commercially available reagents, they can be reprocessed and recycled, they
autonomously heal at room temperature, and they can be hydrolytically degraded at
the end of their service life.
The objective of the second stage was to enhance the performance of dynamic covalent
networks. Starting from the materials and the synthesis processes developed in the
first stage, the trade-off between self-healing/reprocessability and creep resistance was
minimized. Solving this trade-off has been a priority in the field, and it is currently
the main performance challenge of dynamic polymer networks. This was achieved
by combining a dissociative and an associative dynamic covalent chemistry in the
same polymer network. This combination enables the fabrication of materials where
the timescale at which they relax can be designed independently of its mechanical
properties and tailored for the application and lifetime of the material.
Finally, these materials were used in several applications where the dynamics bonds
bring a performance advantage over traditional polymers. The materials were used in
soft robotics, smart textiles, electronic skin, and 3D printing, proving its applicability
in key technologies for the future without giving up on sustainability.
challenges in polymer materials, especially in terms of sustainability. The dynamic
covalent chemistries enhance processability, enable recycling of the reversibly cross-
linked thermosets and elastomers, and offer repairability. Over the last 10 years, the
maturity of these networks has exponentially increased. However, they still haven’t
made it into the mass consumer market.
To stand a chance in the competitive polymer industry, dynamic polymer networks
need to further exploit their advantageous properties and enhanced performance in
combination with a focus on sustainability. This overarching objective has been divided
in three stages, where the results of each stage were sequentially added to the next
one.
The first main focus is sustainability in all its aspects. Dynamic covalent polymer
networks with self-healing properties were developed using the 12 principles of green
chemistry as the designing driving force. The sustainability was tackled from a holistic
point of view, taking into account the whole life cycle of the material (circular economy).
The developed self-healing elastomers account for the sustainability of (1) the raw
materials and (2) solvents, (3) the reusability, (4) the (re)processability, and (5) the end
of life of the material. They are synthesized by a simple one-pot, solventless synthesis
from commercially available reagents, they can be reprocessed and recycled, they
autonomously heal at room temperature, and they can be hydrolytically degraded at
the end of their service life.
The objective of the second stage was to enhance the performance of dynamic covalent
networks. Starting from the materials and the synthesis processes developed in the
first stage, the trade-off between self-healing/reprocessability and creep resistance was
minimized. Solving this trade-off has been a priority in the field, and it is currently
the main performance challenge of dynamic polymer networks. This was achieved
by combining a dissociative and an associative dynamic covalent chemistry in the
same polymer network. This combination enables the fabrication of materials where
the timescale at which they relax can be designed independently of its mechanical
properties and tailored for the application and lifetime of the material.
Finally, these materials were used in several applications where the dynamics bonds
bring a performance advantage over traditional polymers. The materials were used in
soft robotics, smart textiles, electronic skin, and 3D printing, proving its applicability
in key technologies for the future without giving up on sustainability.
| Original language | English |
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| Awarding Institution |
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| Supervisors/Advisors |
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| Award date | 3 Oct 2024 |
| Publisher | |
| Print ISBNs | 9789464948516 |
| Publication status | Published - 2024 |