The design of structurally dynamic molecular networks can offer strategies for fabricating stimuli-responsive adaptive materials. Herein we first report a gas-responsive dynamic gel system based on frustrated Lewis pair (FLP) chemistry. Two trefoil-like molecules with bulky triphenylborane and triphenylphosphine groups are synthesized as complementary Lewis acid and base with trivalent sites. They can together bind CO2 gas molecules and further form a cross-linked network via the bonding interactions between FLPs and CO2 . Such CO2 -bridged dative linkages are shown to be dynamic covalent bonds, which endow the frustrated Lewis network with adaptable behaviors and unprecedented gas-regulated viscoelastic, mechanical, and self-healing performance. This study is an initial attempt to apply the FLP concept in materials chemistry, but we believe that this strategy will open a promising future for gas-sensitive smart materials.
Keywords: carbon dioxide; dynamic covalent bonds; frustrated Lewis pairs; gas responsiveness; molecular networks.
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