Xxxxxx Xxxx X. Xxxxxxxx, Xxxxxx X. Xxxxxxxxx, Xxx Xxx, and Xxxxxxx X. X. Xxxx* Abstract: The creation of adaptive matter is heavily inspired by biological systems. However, it remains challenging to design complex material responses that are governed by reaction networks, which lie at the heart of cellular complexity. The main reason for this slow progress is the lack ofa general strategy to integrate reaction networks with materials. Herein we use a systematic approach to preprogram the response of a hydrogel to a trigger, in this case the enzyme trypsin, which activates a reaction network embedded within the hydrogel. A full characterization of all the kinetic rate constants in the system enabled the construction of a computational model, which predicted different hydrogel responses depending on the input concentration of the trigger. The results of the simulation are in good agreement with experimental findings. Our methodology can be used to design new, adaptive materials of which the properties are governed by reaction networks of arbitrary complexity. Living systems are adaptive and use enzymatic reaction networks to detect changes in their environment, process input information, and determine an appropriate response.[1] Materials science has recently taken a keen interest in the adaptivity of living systems,[2] and has created new materials with life-like properties such as self-healing,[3] camouflaging,[4] and control over surface characteristics.[5] Impressive exam- ples include the incorporation of the oscillating Belousov– Zhabotinsky reaction into a self-walking gel,[6] and the work of Xxxxxxxxx and co-workers,[7] who used chemo–mechanico– chemical feedback loops to produce a homeostatic material. Others have pioneered control over hydrogel lifetimes with preprogrammed feedback loops using organic[8] or enzy- matic[9] reactions. However, progress towards “life-like” materials has been slow as we lack a general framework for constructing materials with autonomous behavior and preprogrammed responses to external stimuli. Designing materials with complex responses requires the incorporation of chemical reaction networks, where the kinetics within the system are suitably balanced.[10] Here, we present a systematic approach to program the complex response of hydrogels, inspired by our previous work on enzymatic reaction networks.[11,12] First, we developed a polyacrylamide (PAAm)-based hydrogel that [*] S. G. J. Xxxxxx, I. N. Vialshin, X. X. Xxxxxxxxx, X. Xxx, Pro...
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