In this work, a facile and simple yet effective method to generate intrinsic autonomous self-healing polymers was developed, leading to new materials that can be easily fine-tuned both mechanically and chemically.

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An efficient strategy to modulate the thermomechanical properties and self-healing of soft polymers has been developed by rationally selecting the metal used for supramolecular crosslinking.

In this paper, a novel self‐healable and stretchable microfluidics system for next generation wearable lab‐on‐a‐chip is presented. An imine‐based precursor with various metal sources (Co(II), Fe(II), and Zn(II)) is used for the development of an intrinsically autonomous self‐healing microfluidic device. Microfluidics fabrication is performed on the self‐healing substrate layer using a mold transfer method. The mechanical properties of the resulting layer are evaluated using tensile strain pull testing. Microfluidic characteristics including fluid flow, wettability, leak, and fluorescence compatibility are investigated to understand its performance in classical microfluidic applications. The new microfluidic devices are also characterized using scanning‐electron microscopy to evaluate the mold transfer capability. The self‐healing microfluidics and the corresponding detailed fluidic characterization presented in this paper will open new opportunities for microfluidic lab on a chip development for various applications, especially in wearable electronics.

A persistent challenge in the field of organic electronics is balancing the optoelectronic properties of π-conjugated semiconducting polymers with their thermomechanical properties. A popular and effective approach to resolve this dichotomy is to blend π-conjugated polymers with amorphous, stretchy elastomers. In this work, poly(diketopyrrolopyrrole-co-thienovinylthiophene) was blended with an easily-prepared poly(dimethylsiloxane)-based phenylurea copolymer (PDMS-PU) to further explore this approach. Interestingly, the differing surface energy and polarity of this soft amorphous copolymer in comparison to other common siloxane-based polymers blended with conjugated polymers showed little impact on the solid-state morphology. Various techniques were used to evaluate the properties of the polymer blends, including atomic force microscopy, UV-vis spectroscopy, and x-ray diffraction. An in-depth morphological evaluation was performed on the blend at varying strain, elucidating the formation of cracks at the nanoscale. The results show a significant decrease in crystallinity and increase in crack onset with increased PDMS-PU content. Fabrication of organic field-effect transistors (OFETs) utilizing the new polymer blends exhibited charge mobility up to 8.2 × 10 −2 cm 2 V −1 s −1 , and charge transfer characteristics up to 75 wt.% PDMS-PU content. The study shows the promise of PDMS-PU/conjugated polymer blends for use in OFETs, and towards the large-scale preparation of mechanically robust and stretchable electronic devices.