Dynamic materials that can sense changes in their surroundings and functionally respond by altering many of their physical characteristics are primed to be integral components of future "smart" technologies. A fundamental reason for the adaptability of biological organisms is their innate ability to convert environmental or chemical cues into mechanical motion and reconfiguration on both the molecular and macroscale. However, design and engineering of robust chemomechanical behavior in artificial materials has proven a challenge. Such systems can be quite complex and often require intricate coordination between both chemical and mechanical inputs and outputs, as well as the combination of multiple materials working cooperatively to achieve the proper functionality. It is critical to not only understand the fundamental behaviors of existing dynamic chemomechanical systems but also apply that knowledge and explore new avenues for design of novel materials platforms that could provide a basis for future adaptive technologies.In this Account, we explore the chemomechanical behavior, properties, and applications of hybrid-material surfaces consisting of environmentally sensitive hydrogels integrated within arrays of high-aspect-ratio nano- or microstructures. This bio-inspired approach, in which the volume-changing hydrogel acts as the "muscle" that reversibly actuates the microstructured "bones", is highly tunable and customizable. Although straightforward in concept, the combination of just these two materials (structures and hydrogel) has given rise to a far more complex set of actuation mechanisms and behaviors. Variations in how the hydrogel is physically integrated within the structure array provide the basis for three fundamental mechanisms of actuation, each with its own set of responsive properties and chemomechanical behavior. Further control over how the chemical stimulus is applied to the surface, such as with microfluidics, allows for generation of more precise and varied patterns of actuation. We also discuss the possible applications of these hybrid surfaces for chemomechanical manipulation of reactions, including the generation of chemomechanical feedback loops. Comparing and contrasting these many approaches and techniques, we aim to put into perspective their highly tunable and diverse capabilities but also their future challenges and impacts.
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