Thermally insulating and sustainable polyolefin foams play an important role in alleviating heat waste. Cyclic olefin copolymer (COC) has remarkable heat resistance and low thermal conductivity, which makes it an excellent candidate as a thermal insulative material. However, COC has critical drawbacks in its foam processing due to low melt strength, which limits its effective application as a thermal insulative material. Herein, we exploit nanofibrillar processing technology to enhance melt strength to develop highly tough and thermally insulating self-reinforced COC composites. The nanofibril network generated by drawing from the COC blends provides dramatic enhancements in the mechanical, rheological and final foam and thermal insulation properties. In particular, this process increases tensile toughness of COC composites by up to twenty-folds higher than neat COC. The results of foam process reveal the presence of COC fibrils in COC matrix improved volume expansion ratio as well as the cell density of the COC composites. Specifically, the expansion ratio of the foams reaches up to 11 with a cell density of 107 cell/cm3, two orders of magnitude higher than that of neat COC foams and thermal conductivity decreased from 0.062 to 0.033 W m−1K−1. As a proof of concept, this work provides a new insight of a self-reinforced approach to develop recyclable, highly tough, and thermally insulative foam.
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