Here we demonstrate direct ink write (DIW) additive manufacturing of carbon nanotube (CNT)/phenolic composites with heat dissipation and excellent electromagnetic interference (EMI) shielding capabilities without curing-induced deformation. Such polymer composites are valuable for protecting electronic devices from overheating and electromagnetic interference. CNTs were used as a multifunctional nanofiller to improve electrical and thermal conductivity, printability, stability during curing, and EMI shielding performance of CNT/phenolic composites. Different CNT loadings, curing conditions, substrate types, and sample sizes were explored to minimize the negative effects of the byproducts released from the cross-linking reactions of phenolic on the printed shape integrity. At a CNT loading of 10 wt %, a slow curing cycle enables us to cure printed thin-walled CNT/phenolic composites with highly dense structures; such structures are impossible without a filler. Moreover, the electrical conductivity of the printed 10 wt % CNT/phenolic composites increased by orders of magnitude due to CNT percolation, while an improvement of 92% in thermal conductivity was achieved over the neat phenolic. EMI shielding effectiveness of the printed CNT/phenolic composites reaches 41.6 dB at the same CNT loading, offering a shielding efficiency of 99.99%. The results indicate that high CNT loading, a slow curing cycle, flexible substrates, and one thin sample dimension are the key factors to produce high-performance 3D-printed CNT/phenolic composites to address the overheating and EMI issues of modern electronic devices.
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