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Chemo-Mechanics of Biodegradable Polymers

Lead Research Organisation: University of Oxford
Department Name: Engineering Science

Abstract

Biodegradable polymers are materials designed to gradually break down into harmless constituents, and eventually disappear after having fulfilled their structural function. They are attracting enormous interest as potential replacements to traditional inert plastics in an attempt to address the plastic pollution problem. Applications include sustainable packaging, agricultural films and fishing nets, among others. Biodegradable polymers are also materials of choice for the design of temporary biomedical implantable devices (e.g. stents, sutures, or orthopaedic fixtures), thanks to their biocompatibility and tunable mechanical properties.

From an engineering design perspective, biodegradable polymers introduce new challenges due to seemingly contradictory requirements: they need to degrade relatively fast after having completed their intended function, but they must also maintain suitable mechanical properties (stiffness, strength, toughness) during service. Addressing these challenges requires a fundamental understanding of the coupled chemo-mechanical effects that dictate the performance of these materials. On the one hand, chemical degradation in water progressively decreases the mechanical properties of the material and causes swelling. On the other hand, mechanical stresses arising from externally-applied loads or geometrical imperfections significantly impact the degradation rate.

The proposed research aims to elucidate the role of mechanics in the chemical degradation of polymers in aqueous environment. This will be achieved by integrating systematic experiments on model polymers (PLA) degrading under loads and new physics-based constitutive models coupling mechanics and chemistry (hydrolysis reaction and diffusion of water and reaction products). The proposed models will be implemented within robust computational tools enabling the in-silico testing of biodegradable components under complex loading conditions up to failure. Ultimately, the research aims to answer the following question: "can we harness mechanical effects to control the degradation rate and failure mode for specific applications?".

The new knowledge, models and computational tools delivered by this project will be directly relevant for a broad range of applications in packaging, engineering and healthcare. Benefits include guidelines for the formulation of polymer systems with targeted mechanical and degradation properties, as well as design guidelines and predictive simulation tools at component level. These will reduce the need for costly and time-consuming trial-and-error experimental approaches, and improve performance and safety of biodegradable devices.
 
Description The work funded through this research led to the development of a novel mathematical model to describe hydrolytic degradation in polymers, which is the dominant degradation pathway in many biodegradable polymers using in medicine, packaging and engineering. The model enables an accurate description of the degradation process at the level of individual chains, while is also suited for simulations of heterogeneous degradation at macroscopic scale. The model was validated by comparing its predictions to a range of experimental data. The degradation model has further been coupled to a viscoplastic constitutive model to predict the effect of degradation on mechanical properties of degradable plastics. The model has been validated by new experimental results for the degradation of PLA. The experimental work also highlighted the effect of mechanical loads on the degradation rate. Ongoing work focuses on the degradation behaviour of PCL for applications in biomedical fibres.
Exploitation Route Theoretical and computational models can be used as a basis for further developments (generalisation or specialisation) in a broad range of problems related to polymer degradation. Our published experimental data can also serve the community in developing new constitutive models for polymers.
Sectors Agriculture

Food and Drink

Healthcare

Manufacturing

including Industrial Biotechology

 
Description DTP (managed by the Department of Engineering Science at the University of Oxford)
Amount £140,000 (GBP)
Funding ID DTP:IDS Research Studentship: Multiphysics modelling of biodegradable polymers 
Organisation Engineering and Physical Sciences Research Council (EPSRC) 
Sector Public
Country United Kingdom
Start 09/2023 
End 03/2027
 
Description International Exchanges 2022 Cost Share (NSFC)
Amount £12,000 (GBP)
Funding ID IEC\NSFC\223221 
Organisation The Royal Society 
Sector Charity/Non Profit
Country United Kingdom
Start 03/2023 
End 03/2025
 
Title Mathematical model of hydrolytic degradation in polymers 
Description The model couples a discrete chain scission model at mesoscale to a continuum reaction-diffusion modelling framework at macroscopic scale, allowing the modelling of heterogeneous degradation by hydrolysis in polymers. The model accounts for various chain scission mechanisms and for autocatalysis. The software implementing the model is freely available to download. 
Type Of Material Computer model/algorithm 
Year Produced 2023 
Provided To Others? Yes  
Impact This model for hydrolytic degradation underpins the development of a more comprehensive modelling framework coupling mechanics and degradation, currently under development in my group. 
URL https://doi.org/10.1016/j.actbio.2023.06.021
 
Description Course for graduate students at the UKACM 2023 conference 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach National
Primary Audience Postgraduate students
Results and Impact I delivered a 2-hour lecture in the graduate school, part of the UKACM2023 conference organised in Warwick (the annual conference of the UK association for computational mechanics). The lecture was intended for the graduate students (approx 200) attending the conference, to broaden their perspectives and expose them to new approaches in solid mechanics. The lecture covered concepts related to chemo-mechanical couplings in materials (polymers and battery materials).
Year(s) Of Engagement Activity 2023
URL https://sites.google.com/view/ukacm2023conference
 
Description Participation at the SCHEMA workshop 
Form Of Engagement Activity Participation in an activity, workshop or similar
Part Of Official Scheme? No
Geographic Reach National
Primary Audience Industry/Business
Results and Impact I participated to SCHEMA Hub Manufacturing Challenge Workshop on Sustainable Elastomers and Plastics. This hub is supported by EPSRC and aims to bring together academia and industry to tackle challenges related to sustainable polymers. About 50 participants attended the workshop. I gave a short talk about my research, which sparked questions and numerous discussions afterwards. I also participated in focused group discussions to identify specific challenges to address within the hub.
Year(s) Of Engagement Activity 2025
URL https://schemahub.ac.uk
 
Description Presentation at an IOM3 technical meeting 
Form Of Engagement Activity Participation in an activity, workshop or similar
Part Of Official Scheme? No
Geographic Reach National
Primary Audience Industry/Business
Results and Impact Presentation of my research in a technical meeting of IOM3 (Institute of Materials, Minerals and Mining) organised by the Elastomer group. The meeting focused on elastomers for biomedical applications, with objective of bringing together academia and industry in this sector. There were about 30 people present in person, and an additional 50 people attending online. Participants included academics, postgraduate students and industry.
Year(s) Of Engagement Activity 2024
URL https://www.iom3.org/resource/elastomers-in-biomedical-devices.html?_gl=1*1g4p8bg*_up*MQ..*_ga*MjM2N...