Catalysis

Ambient Conversion of Carbon Dioxide into Liquid Fuel by a Heterogeneous Synergetic Dual Single-Atom Catalyst

Authors

Abstract

Ambient conversion of carbon dioxide into various liquid fuels or chemicals is a potential economical solution for reducing CO2 emissions, which may be responsible for recent climate change. Here, we report a highly active dual single-Pd-atom catalyst for ambient conversion of CO2 to formic acid using a step-by-step catalyst design strategy by the density functional theory (DFT) method. 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 formic acid under ambient conditions (30 °C, 1 bar) with a turnover frequency (TOF) as high as 13.46 h-1, which is the first such report in the field of heterogeneous catalysts. Two major factors contributing to this extraordinary catalytic activity include a pore enrichment effect of the microporous structures of the covalent triazine framework and a ternary synergetic effect among two neighbouring Pd atoms and rich nitrogen environment. Our work may aid the development of heterogeneous catalysts to produce other commonly used fuels from CO2 under ambient conditions.

Content

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Supplementary material

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Ambient Conversion of Carbon Dioxide into Liquid Fuel by a Heterogeneous Synergetic Dual Single-Atom Catalyst
Supplementary Table and FIgure.