Mechanically Adaptable High‐Performance p(SBMA‐MMA) Copolymer Hydrogel with Iron (II/III) Perchlorate for Wearable Thermocell Applications

Abstract Quasi‐solid‐state thermocells (QTECs) show promise as a power source for wearable devices by converting body heat into electricity. While significant progress has been made with p‐type elements for QTECs, challenges remain with their n‐type counterparts. Here, a high‐performance n‐type QTEC element is presented, using a copolymer hydrogel that outperforms conventional p‐type elements. This copolymer hydrogel combines hydrophilic zwitterionic sulfobetaine methacrylate (SBMA) for ionic conduction and hydrophobic methyl methacrylate (MMA) for structural stability. By increasing the MMA content from 35 to 100 wt.%, versatile control is achieved over the hydrogel's elastic modulus (72 kPa to 127.7 MPa) and tensile strength (54 kPa to 6.7 MPa). A high mechanical toughness of 7.2 MJ m ⁻³ is also achieved at 68 wt.% MMA. The mechanically robust and high toughness p(SBMA‐MMA) hydrogel is then immersed in Fe(ClO ₄ ) _2/3 solutions of different concentrations to evaluate its performance as an n‐type QTEC element. The hydrogel with 0.8 M Fe(ClO ₄ ) _2/3 exhibits a high ionic Seebeck coefficient of −1.7 mV K ⁻¹ , a power density of 1.1 mW m ⁻² K ⁻² , and an elastic modulus of 1.6 MPa, which is similar to that of human skin. Finally, the optimized n‐type p(SBMA‐MMA) hydrogels demonstrate the potential application for wearable devices.