Unraveling the effects of P and S doping over g-C3N4 in strengthening Lewis basicity for CO2/glycerol conversion: A theoretical and experimental study
2023
Fao, Gossa Dare | Catherine, Hepsiba Niruba | Huang, Chun-Hao | Lee, Yi-Lin | Jiang, Jyh-Chiang | Hu, Chechia
Conversion of CO₂ to chemicals and fuels has attracted considerable attention as CO₂ is a nontoxic, non-flammable, and cheap carbon-oxygen source. However, the kinetics of CO₂ conversion into other chemicals remains a challenge due to its thermodynamic stability. Herein, P and S co-doped graphitic-carbon nitride (PSCN) catalyst was synthesized through one-step thermal condensation to improve its Lewis acidity and basicity and investigate carbon dioxide/glycerol (CO₂/GLY) conversion. The catalytic GLY conversion at 210 °C reached 60% and 85% using pristine g-C₃N₄ (CN) and PSCN, respectively, with CO₂ as a carbon feedstock and CH₃CN as a dehydrating agent. Density-functional theory (DFT) calculations revealed that the efficient charge transfer resulting from P and S doping could increase the catalytic activity for CO₂/GLY conversion by lowering the activation barrier. This is the first study to demonstrate the catalytic activity of the PSCN catalyst for the CO₂/GLY conversion and the computational work for the GLY carboxylation reaction. Moreover, the interaction site and adsorption energy were investigated for the adsorption of CO₂ and GLY on PSCN and CN to elucidate the reaction mechanism. Our results demonstrated that PSCN could serve as a superior catalyst and pave new light for CO₂/GLY conversion.
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