Water-Reprocessable, Reformable, and Ecofriendly Sustainable Material Based on Disulfide-Cross-Linked Polyethyleneimine

[Image: see text] A reformable polymer gel material has been developed based on the disulfide cross-linking of low-molecular-weight polyethylenimine (PEI) that can be synthesized through a facile thiolation method and reprocessed through an aqueous method without the use of solvents or additional chemicals. Despite being made with water-soluble PEI, the cross-linked gel shows good mechanical integrity and its properties can be controlled through the fabrication parameters, maintaining the hydrophilic nature of PEI while being sufficiently robust to form a free-standing film that does not dissolve in water. The properties of the gel have been characterized by Fourier transform infrared spectroscopy, thermogravimetry, and dynamic mechanical analyses, showing the effect of parameters such as the degree of thiolation and thermal curing. The reformability of the gel comes from the disulfide cross-links, which can be disrupted and reformed through a simple, aqueous processing method utilizing ultrasonication, creating an aqueous dispersion, which can be recast multiple times with minimal loss in physical properties.