3D-Printable and Robust All-in-One Polymer-Entangled Photocatalytic Microreactors for Visible-Light-Driven Hydrogen Evolution

Hydrogels show promise in preventing inorganic catalysis aggregation during hydrogen evolution. However, the incompatible intrinsic properties of inorganics and hydrogels can cause catalyst release during the reaction. One solution is incorporating polymer photocatalysts into hydrogels, but low photocatalytic efficiency due to anti-synergetic effects between polymers and hydrogels remains a challenge. Herein, we developed all-in-one photocatalytic microreactors (PMRs) with excellent stability and efficiency by strongly entangling polymers with hydrogels and designing heterogeneous hydrogels. This approach prevents catalyst loss while achieving a high hydrogen evolution efficiency, self-healability, and stretchability. Moreover, PMRs maintain their efficiency even after they undergo freeze-drying and rehydration. Remarkably, we demonstrate the construction of PMRs into three-dimensional (3D) structures via 3D-printing at room temperature without additional supporting material. In light of these advantages, we have demonstrated a strategy for rapidly manufacturing PMRs with high stability, reactivity, and 3D-printability, which has significant potential for practical applications. © 2024 American Chemical Society