Nature offers interesting examples of structures with a gradually changing composition that provides unique mechanical properties. Today, the transfer of biological principles to technical applications is gaining increasing attention. One prominent example of the transfer of biomimetic principles to materials science is the mussel byssus. Byssus threads possess gradually changing mechanical properties from soft to stiff in order to efficiently attach the mussel to the rock. This design is the basis for polymer gradient materials. Herein, we give a comprehensive overview of the most recent developments in the field of PGMs. In addition to basic terminology and definitions, selected highlights of PGMs are presented, followed by experimental techniques and characterization methods.magnified image

Poly(dimethyl siloxane) with a compositional gradient was fabricated via a precision syringe pump setup. Stretching of the substrate and subsequent oxygen plasma oxidation resulted in a continuously changing wrinkle wavelength on the surface upon relaxation. This approach is a powerful tool for designing gradient surfaces with tailored topography.

Gradients are a natural design principle in biological systems that are used to diminish stress concentration where materials of differing mechanical properties connect. An interesting example of a natural gradient material is byssus, which anchors mussels to rocks and other hard substrata. Building upon previous work with synthetic polymers and inspired by byssal threads, protein gradient films are cast using glycerine-plasticized gelatine and fibroin exhibiting a highly reproducible and smooth mechanical gradient, which encompasses a large range of modulus from 160 to 550 MPa. The reproducible production of biocompatible gradient films represents a first step towards medical applications.

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Marine mussels use their threads for attachment to any substratum and these biopolymer gradient fibers show an excellent combination of stiff and soft mechanical properties. A straightforward approach for the preparation of macroscopic longitudinal polymer gradient materials on the centimeter scale based on a poly(dimethyl siloxane) system is presented. Compositional gradients are realized by using three syringe pumps feeding different prepolymers capable to undergo thermal cross-linking. Within the gradient samples, the stiffness between the hard and soft part can be varied up to a factor of four. The gradients are analyzed by UV-Vis spectroscopy as well as compressive and tensile modulus testing.