Smart Surfaces with pH-Responsiveness Enhanced by Multiscale Hierarchical Structures Fabricated by Laser Direct Writing

In contemporary applications, smart surfaces capable of altering their properties in response to external stimuli have garnered significant attention. Nonetheless, the efficient creation of smart surfaces exhibiting robust and rapid responsiveness and meticulous controllability on a large scale remains a challenge. This paper introduces an innovative approach to fabricate smart surfaces with strong pH-responsiveness, combining femtosecond laser direct writing (LDW) processing technology with stimulus-responsive polymer grafting. The proposed model involves the grafting of poly(2-diethylaminoethyl methacrylate) (PDEAEMA) onto rough and patterned Au/polystyrene (PS) bilayer surfaces through Au-SH bonding. The incorporation of LDW processing technology extends the choice of microstructures and roughness achievable on material surfaces, while PDEAEMA imparts pH responsiveness. Our findings revealed that the difference in contact angle between acidic and basic droplets on the rough PDEAEMA-g-Au surface (similar to 118 degrees) greatly surpasses that on the flat PDEAEMA-g-Au surface (similar to 72 degrees). Next, by leveraging the precision control over surface microstructures enabled by the LDW processing technique, this difference was further augmented to similar to 127 degrees on the optimized patterned PDEAEMA-g-Au surface. Further, we created two distinct combined smart surfaces with varying wettability profiles on which the hydrophilic-hydrophobic boundaries exhibit reliable asymmetric wettability for acidic and basic droplets. Additionally, we prepared a separator, realizing a better visual distinction between acid and base and collecting them separately. Given the effective abilities found in this study, we postulate that our smart surfaces hold substantial potential across diverse applications, encompassing microfluidic devices, intelligent sensors, and biomedicine.