CO2-fueled non-equilibrium supramolecular gels as gas-encoded information encryption materials

Dissipative self-assembly, which exploits energy inputs of chemical fuels to maintain the functional states far from equilibrium, is essential to living systems. Among a variety of fuels, carbon dioxide (CO₂) gas has yet to be introduced in artificial dissipative materials. Here we describe a CO₂-fueled non-equilibrium co-assembly system that couples with a C1 catalytic pathway to dissipate the fuel for function output. Using common frustrated Lewis pair (FLP) as precursors, CO₂ can dynamically bridge between them to constitute metastable amphiphiles, which not only highly activate CO₂ but also enable their co-assembly with substrates into a transient fibrillar gel. In turn, the backward pathway is realized by cooperative C1 catalysis of the substrate and activated CO₂ species in the assembled state. This can boost the depletion of gas fuel and facilitate disassembly to the sol. Moreover, tailoring the intrinsic substrate/FLP chemistries, as well as external cues, to shift the catalytic activity is accessible to regulate the period and lifetime of sol-gel-sol transition over a wide range. Based on the tunability in phase transition on a time scale, we develop time-gated information encryption materials using the transient FLP array loaded gas-encoded substrates, and the correct information can be read only at a specified time window. This study provides inspiration for a new paradigm of fuel for dissipative systems and their intelligent materials applications.