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Multicomponent hydrogels offer a tremendous opportunity for preparing useful and exciting materials that cannot be accessed using a single component. Here, we describe an unusual multi‐component low‐molecular weight gelling system that exhibits pH‐responsive behavior involving cooperative hydrogen bonding between the components, allowing it to maintain a gel phase across a wide pH range. Unlike traditional acid‐triggered gels, our system undergoes a change in the underlying molecular packing and maintains the β‐sheet structure both at acidic and basic pH. We further establish that autonomous programming between these two gel states is possible by an enzymatic reaction which allows us to prepare gels with improved mechanical properties., We show that a multicomponent supramolecular gel with two opposite ionizable pendant groups on different components can exhibit unusual phase behavior involving cooperative hydrogen bonding between the components, allowing it to maintain a gel phase across a wide pH range. Autonomous programming between these two gel states is possible by an enzymatic reaction which allows the preparation of gels with improved mechanical properties.

(Figure Presented) Extreme chemistry: The carbon nitride imide C 2 N 2 (NH) is synthesized from the single-source precursor 1-cyanoguanidine under high-pressure and high-temperature conditions in a laser-heated diamond-anvil cell. Characterization of single crystals recovered at ambient conditions reveals that the new compound adopts a defect wurtzite structure (see picture). © 2007 Wiley-VCH Verlag GmbH & Co. KGaA.