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Thermoplastic polyurethanes (TPUs) have received considerable attention because of their flexible structure and comprehensive performance. 3,3-Dimethyl-4,4′-diphenyl diisocyanate (TODI) was first introduced to fabricate highperformance TPU by tailoring the mole ratio of the hard segment to the soft segment and the molecular weight of the soft segment for three-dimensional (3D) printing. The influence of the microstructure on glass transition temperature, tensile strength, modulus, loss factor, and softening temperature was investigated. The annealing process was proved to increase the degree of microphase separation of TODI-based TPU. Compared with TPU derived from widely commercialized isocyanates, our prepared TODI-based TPU exhibited remarkably high heat resistance. In addition, it is worth noting that our TODI-based TPU prepolymer has long-term and stable storage, which is beneficial for industrial application. This work is crucial to fabricate new TPU elastomer materials with high heat resistance for 3D printing and evaluate the structure−property behavior of TODI-based TPU, which could help other researchers design TODI-based TPU.

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Petroleum-based polymer materials heavily rely on nonrenewable petrochemical resources, and damping materials are an important category of them. As far as green chemistry, recycling, and damping materials are concerned, there is an urgent need for renewable and recyclable biobased materials with high damping performance. Thus, this study designs and synthesizes a series of polylactic acid-based thermoplastic polyurethanes (PLA-based TPUs) composed of modified polylactic acid polyols, 4,4′-diphenylmethane diisocyanate, and 1,4-butanediol. PLA-based TPUs, as prepared, display excellent mechanical properties, damping performance, and biocompatibility. Otherwise, they can be used for three-dimensional printing (3D printing). Under multiple recycling, the overall performance of PLA-based TPUs is still maintained well. Overall, PLA-based TPUs, as designed in this article, show a potential application in damping materials under room temperature and personalized shoes via 3D printing and could realize resource recycling and material reuse.