Most current hydrogel actuators suffer from either poor mechanical properties or limited responsiveness. Also, the widely used thermo-responsive poly-(N-isopropylacrylamide) (PNIPAM) homopolymer hydrogels have a slow response rate. Thus, it remains a challenge to fabricate thermo-responsive hydrogel actuators with both excellent mechanical and responsive properties. Herein, ultrafast thermo-responsive VSNPs-P­(NIPAM-co-AA) hydrogels containing multivalent vinyl functionalized silica nanoparticles (VSNPs) are fabricated. The ultrafast thermo-responsiveness is due to the mobile polymer chains grafted from the surfaces of the VSNPs, which can facilitate hydrophobic aggregation, inducing the phase transition and generating water transport channels for quick water expulsion. In addition, the copolymerization of NIPAM with acrylic acid (AA) decreases the transition temperature of the thermo-responsive PNIPAM-based hydrogels, contributing to ultrafast thermo-responsive shrinking behavior with a large volume change of as high as 72.5%. Moreover, inspired by nature, intelligent hydrogel actuators with gradient structure can be facilely prepared through self-healing between the ultrafast thermo-responsive VSNPs-P­(NIPAM-co-AA) hydrogel layers and high-strength VSNPs-PAA-Fe3+ multibond network (MBN) hydrogel layers. The obtained well-integrated gradient hydrogel actuators show ultrafast thermo-responsive performance within only 9 s in 60 °C water, as well as high strength, and can be used for more practical applications as intelligent soft actuators or artificial robots.

Poly(vinyl alcohol) (PVA), tannic acid (TA) and sodium hydroxide (NaOH) were used to prepare low-flammability, mechanically-strong aerogels via an environmentally-friendly freeze-drying method. Because of the strong interaction between TA and PVA through hydrogen bonds, PVA/TA/NaOH aerogels exhibited compressive moduli as high as 12.7 MPa, 20 times that of the control PVA aerogel. The microstructure of the aerogels in this study showed that the addition of NaOH disrupted the typical “card of house” aerogel structure, while the samples with TA showed a stereoscopic uniform structure. The thermal stabilities of aerogels were tested by thermogravimetric analysis, showing both a decrease on the onset of decomposition temperature, and a reduction in decomposition rate after initial char formation. The peak heat release rate and total heat release, as measured by cone calorimetry, dropped by 69% and 54%, respectively, after adding TA and NaOH.

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Sodium hydroxide was used as a base catalyst to reduce the flammability of poly(vinyl alcohol) (PVA) aerogels. The base-modified aerogels exhibited significantly enhanced compressive moduli, likely resulting in decreased gallery spacing and increased numbers of “struts” in their structures. The onset of decomposition temperature decreased for the PVA aerogels in the presence of the base, which appears to hinder the polymer pyrolysis process, leading instead to the facile formation of dense char. Cone calorimetry testing showed a dramatic decrease in heat release when the base was added. The results indicate that an unexpected base-catalyzed dehydration occurs at fire temperatures, which is the opposite of the chemistry normally observed under typical synthesis conditions.