Periodic Reporting for period 1 - FuelHydrogel (Constructing chemically fueled hydrogels of polymers)
Reporting period: 2021-11-01 to 2023-10-31
Most synthetic materials are close to or reside in equilibrium, however, life, the most ‘intelligent materials’ on earth, always stays away from equilibrium. This non-equilibrium state is usually sustained by high-energy molecules (chemical fuels) harvested from metabolic reaction cycles. This has inspired the construction of chemically fuelled dissipative molecular assemblies. Currently, these chemically fueled systems mainly focus on small molecules. Compared to small molecules, polymers show advantages in constructing 3D-bulk materials, as well as, integrating and amplifying molecular-scale changes to visible macroscopic changes. We thus propose to extend the construction of dissipative assemblies from small molecules to polymers. The overall goal of the ´FuelHydrogel´ project is to construct chemically fuelled dissipative materials of polymers (polysaccharides) which are regenerative and accessible to spatiotemporal control. This new generation of materials could be used to address our challenges in materials chemistry and biomedicine. Moreover, this action will extend the research domain of systems chemistry from small molecules to polymers.
During the implementation of the project, we have achieved important progress in research and dissemination.
The development of suitable activation/deactivation reaction cycles for polysaccharides is the crucial core part of the project. The activation reaction should be a reaction lead to the chemical modification of the polysaccharides for the generation of hydrogels or nanogels and the deactivation should be the simultaneous hydrolysis of the modified polysaccharide back to the original polymer. We thus designed and investigated a set of activation/deactivation reactions in small molecules as the model systems and which allow us to test a wide range of chemical reactions and coupling reagents to identify the reactions and products. We also tested two of activation/deactivation reactions on polysaccharides directly. We found that one of the reactions and the hydrolysis of the resulting product can progress under the same condition, indicating these reactions can be used to construct the reaction cycles for making the chemically fueled polysaccharide-based hydrogels although the suitable reaction conditions still need further screening.
To strengthen the dissemination of our research and systems chemistry, I have carried out some dissemination and outreach activities with my supervisor.
The development of suitable activation/deactivation reaction cycles for polysaccharides is the crucial core part of the project. The activation reaction should be a reaction lead to the chemical modification of the polysaccharides for the generation of hydrogels or nanogels and the deactivation should be the simultaneous hydrolysis of the modified polysaccharide back to the original polymer. We thus designed and investigated a set of activation/deactivation reactions in small molecules as the model systems and which allow us to test a wide range of chemical reactions and coupling reagents to identify the reactions and products. We also tested two of activation/deactivation reactions on polysaccharides directly. We found that one of the reactions and the hydrolysis of the resulting product can progress under the same condition, indicating these reactions can be used to construct the reaction cycles for making the chemically fueled polysaccharide-based hydrogels although the suitable reaction conditions still need further screening.
To strengthen the dissemination of our research and systems chemistry, I have carried out some dissemination and outreach activities with my supervisor.
I discovered several new reactions which show high potential to be used to build chemically fueled polysaccharide-based materials. These new reactions are efficient and can also be used for all kinds of chemical modification and functionalization of polysaccharides and other polymers. With the support of MSCA fellowship, we have taken important steps to extend the research domain of systems chemistry from small molecules to polymers.