Electroreduction of Carbon Dioxide in Metallic Nanopores through a Pincer Mechanism

다국어 초록 (Multilingual Abstract)

Metallic catalysts with nanopores are advantageous on improving both activity and selectivity, while the reason behind that remains unclear all along. In this work, porous Zn nanoparticles (P‐Zn) were adopted as a model catalyst to investigate the catalytic behavior of metallic nanopores. In situ X‐ray absorption spectroscopy, in situ Fourier transform infrared spectroscopy, and density functional theory (DFT) analyses reveal that the concave surface of nanopores works like a pincer to capture and clamp CO2 and H2O precursors simultaneously, thus lowering the energy barriers of CO2 electroreduction. Resultantly, the pincer mechanism endows P‐Zn with a high Faradic efficiency (98.1 %) towards CO production at the potential of −0.95 V vs. RHE. Moreover, DFT calculation demonstrates that Co and Cu nanopores exhibit the pincer behavior as well, suggesting that this mechanism is universal for metallic nanopores.
In situ analytic techniques and theoretical calculations were employed to investigate the electroreduction of CO2 in metallic nanopores. It was found that the concave surface of metallic nanopores works like a pincer to capture and clamp CO2 and H2O precursors simultaneously, thus lowering the energy barriers of CO2 electroreduction.