Abstract
Dissipative self-assembly, which exploits energy inputs of chemical fuels to maintain the functional states far from equilibrium, is essential to the living systems. Among a variety of fuels, carbon dioxide (CO2) gas, as one of the most ubiquitous but original forms of fuel on which life depends, has yet been introduced in artificial dissipative materials. Here we describe a CO2-fueled non-equilibrium co-assembly system that couples with a C1 catalytic feedback path to drive fuel dissipation and 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 feedback process is realized by cooperative C1 catalytic insertion owing to the proximity of substrate and activated CO2 species in the assembled state. This can boost the depletion of gas fuel and facilitate disassembly to 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-dependent 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 on a new fuel paradigm for dissipative system and their intelligent material applications.