Intrinsically Colored and Luminescent Silk

A IO N Silk has been a highly prized material since its discovery a few thousand years ago, with a current annual industrial output of approximately 30 billion US dollars in China alone. [ 1 , 2 ] In silk industry, the outer layer of silk (sericin) needs to be removed in order to use the core of silk (fi broin) that has excellent mechanical properties combined with luster, smoothness, and comfort. To impart color to the fi nished products, silk fi broin is subjected to the dyeing process including steps to remove excess dye molecules and to restore the properties of silk that are altered due to the harsh conditions involved in the process. [ 3 ] Here, we demonstrate an in vivo uptake of dyes into domesticated silkworms, leading to the direct production of intrinsically colored silk by the silkworms. The biological incorporation of dyes into silk fi broin is a greener method of producing colored silk because it eliminates the need for an external dyeing process, along with the resources (water, energy, additional chemicals) and post-treatments associated with it. A series of fl uorescent dyes were successfully used as model compounds to investigate and understand their selective uptake into fi broin or sericin through fl uorescence imaging and spectroscopic quantifi cation. A better understanding of the molecular factors that determine the uptake of substances into silk fi broin was established to select and design appropriate molecules for producing intrinsically colored and luminescent silk fi broin, i.e., by controlling the structure-dependent hydrophobicity and self-assembly capability of these molecules. In addition to the production of intrinsically colored silk for textile applications, the current work also results in a biocompatible and luminescent silk scaffold that allows better visualization of cells and monitoring of the scaffold performance over time. When applied to other compounds with similar molecular properties, this process can potentially lead to functional silk for various biomedical applications including tissue engineering and bioelectronic, bio-optic, and biomicrofl uidic devices. [ 4–6 ]