Fig. 3: Mechanistic insights into the electrocatalytic CO2RR on CoPc-based electrodes.

In situ SERS of the a CoPc/ppy/GDE and b CoPc/CNT-GDE under applied bias ranging from −0.4 to −1.4 V versus RHE in CO2-saturated 0.1 M KHCO3. There is no iR correction for voltages. c The ratio of Co+: Co2+ during CO2RR under applied bias ranging from the −0.4 to −1.4 V versus RHE during CO2RR. d In situ ATR-SEIRAS spectra of CoPc/ppy/GDE collected in CO2-saturated 0.1 M KHCO3 with an H-type cell, the potential was applied from −0.4 to −0.8 V versus RHE. There is no iR correction for voltages. e EXAFS spectra of CoPc/ppy/GDE polarized at −0. 8 V versus RHE in CO2-saturated 0.1 M KHCO3 for different reaction periods; commercial CoPc was used as the reference. There is no iR correction for voltages. Note that these spectra were collected under ex situ conditions, during the CO2-to-CO conversion the CoPc/ppy/GDE electrode was taken out from the electrochemical cell at designated time and subjected to measurements. Source data are provided as a Source Data file. f Calculated free energy diagrams for CO2RR on CoPc/ppy/GDE and CoPc/GDE. Raw computational and simulation data are provided as Source Data and Supplementary Data 1.