New Article: Recyclable, self-strengthening starch-based epoxy vitrimer facilitated by exchangeable disulfide bonds

A new article out of Ning Yan’s lab has been published in the Chemical Engineering Journal about a self-strengthening, recyclable, starch-based epoxy vitrimer written by Nicole Tratnik, Nicolas R. Tanguy, and Ning Yan.

Click here to view the full article for free until October 5th, 2022.


Epoxy vitrimers have emerged as a new class of self-healing, recyclable, and reprocessable materials, offering new opportunities to traditional epoxy thermosets by improving life-span, while providing additional functionalities. Nevertheless, retaining 100 % of the original mechanical performances remains difficult for vitrimers after several reprocessing cycles due to progressive changes in the vitrimer networks during rearrangements. In this study, we designed a novel epoxy vitrimer with a higher renewable content compared to conventional epoxies by using renewable materials. The bio-based epoxy vitrimer was synthesized from epoxidized starch amylopectin together with diallyl disulfide, that is naturally found in garlic, and a thiol (pentaerythritol tetrakis(3-mercaptopropionate) (PETMP)). Diallyl disulfide and PETMP enabled the formation of a recyclable, and reprocesseable, vitrimer network. The epoxy vitrimer displayed unprecedented self-strengthening after 5 recycling cycles (tensile strength increased over 900 %) caused by the mechanically-induced homogeneization of the diallyl disulfide/thiol and the starch epoxy ghost granule phases during the recycling process, thereby increasing the vitrimer cross-linking density during reformation. Reprocessing the vitrimer 5-times improved the mechanical and thermal properties, raising glass transition temperature, Young’s modulus, and tensile strength from 7 °C to 25 °C, 2.98 MPa to 268 MPa, and 1.87 MPa to 18.47 MPa, respectively. Hence, capitalizing on mechanically-induced phase homegeneization during the vitrimer reprocessing, this work introduces a strategy for the design of self-strengthening bio-based and recyclable thermosets.