Abstract
Despite great progress in the active interfacing between various abiotic materials and living organisms, the development of a smart polymer matrix with modulated functionality of algae towards the application of green bioenergy is still rare. Herein, we design a thermally sensitive poly(N-isopropylacrylamide)-co-poly(butyl acrylate) with an LCST (ca. 25 °C) as a chassis, which could co-assemble with algal cells based on hydrophobic interaction to generate a new type of robust hybrid hydrogel living material. By modulating the temperature to 30 °C, the volume of the polymer matrix is shrunk by 9 times, which allows the formation of physical shading and metabolism changing of the algae, and then triggers the functionality switching of the algae from photosynthetic oxygen production to hydrogen production. By contrast, by decreasing the temperature to 20 °C, the hybrid living materials go into a sol state where the algae behave normally with photosynthetic oxygen production. In particular, due to the proliferation of the algae in living materials, a long-term and exponential enhancement in the amount of hydrogen produced is achieved. Overall, it is anticipated that our investigations could provide a new paradigm for the development of polymer/living organism-based hybrid living materials with synergistic functionality boosting green biomanufacturing.