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Rapidly Responding pH- and Temperature-Responsive Poly (N-Isopropylacrylamide)-Based Microgels and Assemblies.

ABSTRACT: Rapidly responding stimuli-responsive materials can have a benefit in a myriad of applications, for example, sensing and biosensing, actuation, and in drug delivery systems. Thermo- and pH-responsive materials have been among the most widely studied, and can be triggered at physiologically relevant temperatures and pH. Here, we have used a "homologous series" of acids based on the acrylic acid (AAc) backbone and incorporated them into N-isopropylacrylamide (NIPAm)-based microgels. Specifically, the acids used were AAc, methacrylic acid (MAAc), ethylacrylic acid (EAAc), and butylacrylic acid (BAAc), which have pK _a's in the range of 4.25-7.4. The resultant microgels were characterized by optical microscopy, and their responsivity to temperature and pH studied by dynamic light scattering. The microgels were subsequently used to generate optical devices (etalons) and their pH and temperature response was also investigated. We found that the devices composed of BAAc-modified microgels exhibit unusually fast response kinetics relative to those of the rest of the devices. We also found that the speed of the response decreased as the length of the acid pendant group decreased, with AAc-modified microgel-based devices exhibiting the slowest response kinetics. Finally, we showed that the kinetics of the device's temperature response also decreased as the length of the acid pendant group decreased, which we hypothesize is a consequence of the hydrophobicity of the acid groups, that is, increased hydrophobicity leads to faster responses. Understanding this behavior can lead to the rational design of fast responding materials for the applications mentioned above.

SUBMITTER: Ahiabu A

PROVIDER: S-EPMC6640923 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:In this paper, we report detailed experimental observations of unusual changes in the thickness of solid poly(N-isopropylacrylamide) (PNIPAM) ultrathin films, which are well known to have temperature-responsive hydrophilic-hydrophobic switching properties. To date, a number of studies have been carried out on the bulk and the brush forms of PNIPAM in contact with liquid water, as well as in highly humid environments, and, recently, these ultrathin films have been preliminarily shown to exhibit temperature responses even under low-humidity, ambient conditions. In this work, the thicknesses of ultrathin PNIPAM films in a temperature/moisture-controlled sample stage were monitored continuously using multichannel X-ray reflectometry. At room temperature, the sample thickness showed an unexpected increase after thermal treatment at 70 °C for 3 h. In the temperature cycle between 15 and 60 °C, heating and cooling resulted in some clear differences. During cooling, initially, the thickness was almost constant but began to increase when the temperature exceeded 33 °C, which corresponds to the lower critical solution temperature (LCST). This observation indicates that the PNIPAM ultrathin film is sensitive to the small amounts of water contained in the air, even under ambient, low-humidity conditions. On the other hand, during heating run from 15 to 60 °C, the humidity dependence was monotonic, and no specific changes in the PNIPAM films were observed at around the LCST. By studying the humidity dependence, we found that the hydrophilic and hydrophobic states of the PNIPAM ultrathin film exhibit different temperature dependence behaviors. In addition, we found that swelling takes place even under low-moisture conditions. To understand the difference in the thickness changes observed on cooling and heating further, some models considering the effect of the boundary conditions in the polymer ultrathin film system were considered. In the case of the ultrathin film, the hydrophilic/hydrophobic switching property occurred only in the surface layer, which dominated the absorption of water molecules from air. In contrast, the interface layer was time-stable and provided an escape route for water molecules during heating.

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Rapidly Responding pH- and Temperature-Responsive Poly (N-Isopropylacrylamide)-Based Microgels and Assemblies.

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