Abstract
Nanosized biomimetics prepared by the strategy of molecular imprinting, that is, the stamping of recognition sites by means of a template-assisted synthesis, are demonstrating potential as plastic antibodies in medicine, proving effective for cell imaging and targeted therapies. Most molecularly imprinted nanoparticles (MIP-NPs) are currently made of soft matter, such as polyacrylamide and derivatives. Yet, MIP-NPs biocompatibility is crucial for their effective translation into clinical uses. Here, we propose the original idea to synthesize fully biocompatible molecularly imprinted nanoparticles starting from the natural polymer silk fibroin (MIP SF-NPs), which is nontoxic and highly biocompatible. The conditions to produce MIP SF-NPs of different sizes (dmean ∼ 50 nm; dmean ∼ 100 nm) were set using the response surface method. The stamping of a single, high affinity (KD = 57 × 10–9 M), and selective recognition site per silk fibroin nanoparticle was demonstrated, together with the confirmation of nontoxicity. Additionally, MIP SF-NPs were used to decorate silk microfibers and silk nanofibers, providing a general means to add entailed biofunctionalities to materials.
Highlights
The development of functional materials capable of binding target molecules with high affinity and selectivity, in vitro and in vivo, continues to be of prime interest for medicine, sensing, and bioengineering
The synthesis of Molecularly imprinted polymers (MIPs)-NPs starting from natural polymers could represent the frontier in nano/materials research, allowing the targeting of additional and specific biological responses, and fully embodying the biomimicry principles
As a notable advantage, imprinting silk fibroin involves the whole range of amino acid side chains present on the fibroin backbone to potentially interact with the template
Summary
The development of functional materials capable of binding target molecules with high affinity and selectivity, in vitro and in vivo, continues to be of prime interest for medicine, sensing, and bioengineering. Whether biocompatible alternatives to the actual set of materials to be stamped are available is still an open question In this respect, Klaus Mosbach,[13] in a pioneer work demonstrated the modification of the specificity of the active site of an enzyme by its partial unfolding followed by refolding in the presence of a non-natural substrate, setting the principle that a protein can be imprinted. Klaus Mosbach,[13] in a pioneer work demonstrated the modification of the specificity of the active site of an enzyme by its partial unfolding followed by refolding in the presence of a non-natural substrate, setting the principle that a protein can be imprinted It was shown how polymers, which are referred to as macromolecular monomers, can be successfully imprinted, including natural materials, such as chitosan and alginates.[14−16] Frequently, these macromolecular monomers have been chemically modified with reactive double bonds so that the formed MIP. 94.6 ± 1.3 nm (PDI 0.35 ± 0.01) when prepared from 0.3% SF-MA (dotted line). (C) SEM image of a single SF-NP (0.3% w/v)
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