Abstract
The bottom-up construction of leaf-like materials capable of using visible light and water to produce oxygen and chemical energy is a major goal of artificial photosynthesis. In this work, we show that robust artificial cells (protocells) prepared by the membranization of polymer/nucleotide coacervate droplets with a bio-inspired Ru-based polyoxometalate (POM) catalytic oxygen-evolving center are capable of continuous light-assisted water oxidation at room temperature. We present a method to electrostatically assemble millions of the photocatalytic protocells into tissue-like protocellular sheets and spheroids and demonstrate that the protocellular assemblies exhibit enhanced rates of photocatalytic water oxidation compared with individual protocells. Our results highlight opportunities for synergistically integrating key aspects of photocatalysis, cytomimetics, and bottom-up engineering toward the development of modular photosynthetic active matter and applications in artificial photosynthesis and energy capture.