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Schematic diagram of microgel/SA composite spherical granular hydrogel formation.

In this work, poly(vinyl alcohol) (PVA) was incorporated into the networks of polyacrylamide/polyacrylic acid (PAM/PAA) to prepare novel PAM/PAA/PVA Triple-network (TN) hydrogels by an in situ polymerization and repeated freezing-thawing (F-T) process. The TN hydrogels have not only high mechanical strength, but also a moderate swelling ability by varying the weight ratio of calcium chloride (CaCl 2 ) and PVA and free shaping. The compressive stress of the as-prepared hydrogels could reach 11 MPa, and the highest stretching stress could reach 0.8 MPa. Upon mechanical loading, the coordination network between PAA and CaCl 2 served as sacrificial bonds to efficiently dissipate energy. However, they can reform when the mechanical load is released, resulting from the fast coordination between PAA and Ca 2+ . Therefore, TN hydrogels have potential application in biomaterials.Scheme 1 Preparation of TN gels by using one-pot, two step method.6790 | RSC Adv., 2018, 8, 6789-6797This journal is

Abstract.A novel post-crosslinking method by heating the composite polymer with dispersed reactive microgels was used to prepare microgel composite (MC) hydrogels. This MC hydrogels were crosslinked by reactive microgels instead of traditional crosslinkers. The reactive microgels contained hydroxymethyl groups, which acted as post-crosslinkers. They were prepared by inverse emulsion polymerization. The formed MC hydrogels at appropriate conditions had high equilibrium swelling ratio and excellent mechanical properties. The heating conditions and the polymer water content influenced the hydrogel properties. For MC hydrogels prepared by direct heating the as-prepared composite polymers with 75% water content, their properties were influenced by heating conditions. When the heating conditions were 90°C for 4 h, the MC hydrogel had a tensile strength of 32 kPa and a high elongation of 960%. In addition, for MC hydrogels prepared by heating the partly evaporated composite polymers, their properties can be adjusted by the polymer water content. Appropriate reduction of the polymer water content was beneficial to improve the mechanical strength of the MC hydrogels. The appropriate polymer water content was important to prepare MC hydrogels with excellent mechanical properties. When the composite polymer with 50% water content was heated at 90°C for 3 h, the MC hydrogel had high tensile strength of 130 kPa and high tensile elongation of 503%.

Acrylamide co 2‐acrylamido‐2‐methylpropane sulfonic acid microgel composite (MC) hydrogels were prepared by heating MC polymer with 50% water content. Crosslinking reaction occurred in the heating process and reactive microgels with hydroxymethyl groups introduced by N‐methylolacrylamide (NMA) were used as postcrosslinkers. Microgel swollen size is influenced by NMA content. Both microgel and its NMA content affect MC hydrogel properties, which relates to the crosslinking chain length and the crosslinking density. The tensile strength of MC hydrogels increases and their elongation decreases as the microgel content increases from 0.1 to 0.5 g. Both the tensile strength and the elongation decrease as the microgel content further increases from 0.5 to 1.1 g. The MC hydrogel tensile strength increases and the elongation decreases as the NMA content of microgels increases from 5.0 to 14.8%. However, they both decrease when the NMA content of microgels exceeds 14.8%. Although the crosslinking chains υ calculated from tensile stress–strain curves were very high, MC hydrogels were elastic and had the highest tensile strength of 127 kPa and considerably moderate elongation of 427%. Their excellent mechanical properties attributed to their unique structure crosslinked by microgel particles. POLYM. COMPOS., 2012. © 2011 Society of Plastics Engineers