This work provides a promising molecular engineering route to construct high performance photonic ionic conductors towards advanced ionotronic applications. Moreover, due to their liquid-free nature, the PIEs exhibit extraordinary stability and durability, which could withstand extreme conditions including both high and low temperatures as well as high humidity. Meanwhile, the synchronous electrical and optical output under mechanical strains could be achieved in the PIEs with the presence of dissociated ions contributed by lithium bond and non-close-packed SiNPs stabilized by hydrogen bond. In virtue of lithium bonding between lithium ions and carbonyl groups in the polymer matrix as well as hydrogen bonding between silanol on the surface of silica nanoparticles (SiNPs) and ether groups along polymer chains, the PIEs demonstrate mechanical strength up to 4.3 MPa and toughness up to 8.6 MJ m −3. Here, we break the limitations through introducing synergistic effect of lithium and hydrogen bonds into an elastomer. However, fabricating PIEs with simultaneous mechanical robustness, good ionic conductivity and brilliant structure color still remains challenging.
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