TY - JOUR

T1 - Double physical network hydrogels with rapid self-recovery and multistimuli-responsive shape memory effects based on low-methoxyl pectin and host-guest interactions

AU - Cai, Tingting

AU - Liu, Xingxun

AU - Blennow, Andreas

AU - Shao, Chuyin

AU - Sun, Weixiang

AU - Tong, Zhen

AU - Wang, Tao

N1 - Publisher Copyright: © 2023

PY - 2024

Y1 - 2024

N2 - Double physical network (DPN) hydrogels exhibit superior performance compared with other hydrogel types due to their unique crosslinking structure. However, certain mechanical properties, such as self-recovery and fatigue resistance, still need improvement, and stimuli-responsiveness can be expanded for a wider range of applications. In this study, we presented a facile strategy for designing multifunctional DPN hydrogels based on a poly-cyclodextrin (PCD) and adamantane (Ad) host-guest supramolecular crosslinked polyacrylamide (PAAm) network and a low-methoxyl pectin (LMP) network established through Ca2+ or H+. ‘Egg box’ junction zones between Ca2+ and COO− on the LMP chains, as well as hydrogen bonding and hydrophobic association junction zones, could be formed during this process. The synergistic effect of the flexible supramolecular network and the stiff LMP network imparted remarkable stress tolerance, fatigue resistance, ductility, and anti-piercing capacities to the DPN hydrogels. The thermal reversible DPN structure also endowed the hydrogel with thermal-accelerated rapid self-recovery, as the hydrogel can virtually recover to its original state within 40 min at 80 °C. Multistimuli-responsive including chemical- and thermal-induced shape memory behavior was achieved based on the versatile LMP network. The temporary shape of the LMP hydrogel could be fixed with the introduction of Ca2+ or H+, while spontaneous shape recovery was observed under near infrared (NIR) radiation or immersion in K2CO3 or NaOH solutions, respectively. Additionally, the DPN hydrogels exhibited notable self-healing behavior when the cut surfaces were contacted and stored at 80 °C. More importantly, green natural resources derived raw materials of cyclodextrin (CD) and LMP also offered a sustainable strategy to prepare functional hydrogels. The combination of the above features of the LMP DPN hydrogel provided a new method for designing smart materials with ideal functions for soft actuators and biomedical applications.

AB - Double physical network (DPN) hydrogels exhibit superior performance compared with other hydrogel types due to their unique crosslinking structure. However, certain mechanical properties, such as self-recovery and fatigue resistance, still need improvement, and stimuli-responsiveness can be expanded for a wider range of applications. In this study, we presented a facile strategy for designing multifunctional DPN hydrogels based on a poly-cyclodextrin (PCD) and adamantane (Ad) host-guest supramolecular crosslinked polyacrylamide (PAAm) network and a low-methoxyl pectin (LMP) network established through Ca2+ or H+. ‘Egg box’ junction zones between Ca2+ and COO− on the LMP chains, as well as hydrogen bonding and hydrophobic association junction zones, could be formed during this process. The synergistic effect of the flexible supramolecular network and the stiff LMP network imparted remarkable stress tolerance, fatigue resistance, ductility, and anti-piercing capacities to the DPN hydrogels. The thermal reversible DPN structure also endowed the hydrogel with thermal-accelerated rapid self-recovery, as the hydrogel can virtually recover to its original state within 40 min at 80 °C. Multistimuli-responsive including chemical- and thermal-induced shape memory behavior was achieved based on the versatile LMP network. The temporary shape of the LMP hydrogel could be fixed with the introduction of Ca2+ or H+, while spontaneous shape recovery was observed under near infrared (NIR) radiation or immersion in K2CO3 or NaOH solutions, respectively. Additionally, the DPN hydrogels exhibited notable self-healing behavior when the cut surfaces were contacted and stored at 80 °C. More importantly, green natural resources derived raw materials of cyclodextrin (CD) and LMP also offered a sustainable strategy to prepare functional hydrogels. The combination of the above features of the LMP DPN hydrogel provided a new method for designing smart materials with ideal functions for soft actuators and biomedical applications.

KW - Double physical network hydrogel

KW - Host-guest interaction

KW - Low-methoxyl pectin

KW - Multistimuli-responsive shape memory

KW - Self-recovery

U2 - 10.1016/j.susmat.2024.e00892

DO - 10.1016/j.susmat.2024.e00892

M3 - Journal article

AN - SCOPUS:85187228239

VL - 40

JO - Sustainable Materials and Technologies

JF - Sustainable Materials and Technologies

SN - 2214-9937

M1 - e00892

ER -