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

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.

Automated summary

The study introduces a new operational strategy to achieve high selectivity and efficiency in solar-driven photoelectrochemical carbon dioxide reduction by designing a high-pressure artificial photosynthetic device. The strategy, quantitatively described by the Langmuir mechanism, demonstrated CO2 reduction selectivity higher than 80% and solar-to-chemical energy conversion efficiency exceeding 0.9%. Additionally, the material and synthesis versatility of this strategy was showcased, shedding new light on selective and efficient catalytic conversions.