A high-pressure artificial photosynthetic device: pumping carbon dioxide as well as achieving selectivity

Abstract

Controlling the products, i.e. achieving high selectivity, is essential yet challenging for many chemical processes. So far, ex/in situ methods have been reported to prepare selective catalysts; here, we present a distinct operational strategy. To demonstrate its power and simplicity, a high-pressure artificial photosynthetic device (HiPAD) was designed correspondingly to achieve selective and efficient solar-driven photoelectrochemical (PEC) carbon dioxide reduction (CO₂R). The HiPAD features a high-pressure operation to enhance the CO₂ concentration, as well as straight operations of copper (Cu) catalyst synthesis and Cu-catalyzed PEC CO₂R to enhance the active site concentration. This strategy is quantitatively described by the Langmuir mechanism. By leveraging it, CO₂R selectivity higher than 80% and solar-to-chemical energy conversion efficiency exceeding 0.9% were experimentally demonstrated. The material and synthesis versatility feature of this strategy was also demonstrated. These results shed new light on selective and efficient catalytic conversions.