Resource-Efficient Interfacial Enzymatic Coloration of Silk Using a Recyclable D5-Mediated Microscale Water-Based Dyeing Platform

Enzyme-catalyzed textile coloration enables in situ chromophore generation under mild conditions. However, aqueous enzymatic coloration often requires high liquor ratios, raising water and enzyme consumption. In this study, we developed a decamethylcyclopentasiloxane (D5)-mediated microscale water-based dyeing platform that promotes chromophore generation at the silk interface and allows continuous-medium recovery and reuse. Silk was pre-impregnated with laccase, and 2,5-diaminobenzenesulfonic acid (DABSA) and gallic acid were employed as representative aromatic amine and polyphenolic precursors. Oxidative coupling produced conjugated chromophoric oligomers. For DABSA, at the same monomer dosage of 3% owf and total laccase dosage, the K/S value increased from 1.11 in water to 10.37 in the D5-mediated platform. Furthermore, 3% owf monomer in D5 matched the color depth of 10% owf in water. The fabrics dyed using the D5-mediated dyeing platform exhibited colorfastness comparable to that of their aqueous-dyed counterparts and showed antibacterial, antioxidant, and UV-protective activities. D5 recovery averaged approximately 93%, with stable coloration over 30 cycles. At comparable color depth, normalized water input, effective laccase input, monomer dosage, and estimated residual-liquid output fell to 10, 5, 30, and 16.65% of aqueous-process values, respectively. This resource-efficient strategy concurrently enables chromophore synthesis, dyeing, functionalization of silk, and solvent recovery within a single integrated process.