摘要
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(CO_(2))gas has yet to be introduced in artificial dissipative materials.Here we describe a CO_(2)-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,CO_(2)can dynamically bridge between them to constitute metastable amphiphiles,which not only highly activate CO_(2)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 CO_(2)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.
基金
supported by the National Natural Science Foundation of China(22371053,21674022,223B2103,51703034)
the National Defense Science and Technology Innovation Zone(166 Program)
the Outstanding Young Scholar Program。
