Ambient hydrogenation of carbon dioxide into liquid fuel by a heterogeneous synergetic dual single-atom catalyst

Abstract

Ambient hydrogenation of CO2 into liquid fuels is a potential economical solution for reducing CO2 emissions. Here, we report a highly active dual single-Pd-atom catalyst for ambient hydrogenation of CO2 to formate using a step-by-step catalyst design strategy. The theoretically predicted catalyst is synthesized experimentally and verified to capture a significant amount of CO2 (5.05 mmol/g, 273 K), and it can efficiently convert CO2 to formate under ambient conditions with a turnover frequency (TOF) as high as 13.46 h–1. Two major factors contributing to this extraordinary catalytic activity include the pore enrichment effect of the microporous structures and the ternary synergetic effect among two neighboring Pd atoms and the rich nitrogen environment. Our work may aid the development of heterogeneous catalysts to produce other commonly used fuels from CO2 under ambient conditions.