Mineral Tanning‐Inspired Metal Ions Coordination Hydrogels with Outstanding Mechanical Strength and Toughness for Flexible Force Sensors

Abstract By virtue of reversible energy dissipation and good ionic conductivity, metal ions have been extensively introduced to construct hydrogels. However, the traditional soaking method to prepare metal ions coordination hydrogels (MI‐HG) faces the challenge of diffusion and combination of metal ions, leading to weak mechanical properties. Inspired by the leather mineral tanning mechanism, a strategy that controls the accessibility of hydrogels by pickling and basifying processes thus significantly improving the strength and toughness of MI‐HG is proposed. To achieve this, polyvinyl alcohol/poly(acrylamide‐co‐acrylic acid) (PVA/PAM‐co‐PAA) hydrogels‐bearing ligands similar to those of leather collagen are fabricated. Zr 4+ , Cr 3+ , Al 3+ , and Fe 3+ commonly used for mineral tanning are chosen as the metal source. The results demonstrate that the mechanical properties of the products (MI‐HG Tanning ) are significantly promoted, especially for Cr 3+ and Zr 4+ . For example, the tensile strength of Zr‐HG Tanning and toughness of Cr‐HG Tanning reach 7.79 ± 0.41 Mpa and 28.01 ± 3.1 MJ m −3 , approximately three and seven times that of their soaking samples. From macro to micro characterization and by theoretical simulation, the mineral tanning mechanism of metal ions first permeating and then effectively combining with carboxylates, thus improving the mechanical performance of MI‐HG Tanning is deciphered, the products of which are promised applications in flexible force sensors.