Journal
CHEMICAL ENGINEERING JOURNAL
Volume 431, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2021.134171
Keywords
CO2 electroreduction; Cu-BTC; Cu@Cu2O; In-situ ATR-FTIR
Categories
Funding
- National Natural Science Foundation, China [51676171]
- Zhejiang Provincial Key Research and Development Program, China [2020C01135]
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A novel MOF-derived Cu@Cu2O heterogeneous electrocatalyst was proposed for improving the Faradaic efficiency of CO2 reduction to methanol, with moderate intermediates adsorption. The presence of a distinct interface between Cu and Cu2O, along with Cu-0/Cu+ and OH on catalyst surfaces, facilitated the hydrogenation reduction of CO2 to methanol. The most favorable reduction route of CO2 to methanol was identified, with the electrocatalyst exhibiting a high peak FECH3OH attributed to synergistic effect between Cu-0 and Cu+ active sites.
To improve Faradaic efficiency (FE) of CO2 reduction reaction (CO2RR) to methanol over Cu-based complex electrocatalysts, a novel MOF-derived Cu@Cu2O heterogeneous electrocatalyst with moderate intermediates adsorption was proposed for highly selective reduction of CO2 to methanol. XRD and HRTEM confirmed the presence of a distinct heterogeneous interface between Cu and Cu2O, while XPS verified the existence of Cu-0/Cu+ and OH on catalyst surfaces. Cu-0/Cu+ with a moderate CO* binding energy and OH which favored H* adsorption were conducive to hydrogenation reduction of CO2 to methanol. The intermediate products CO*, COOH*, and CHO* were detected on in-situ electrochemical ATR-FTIR spectroscopy. The most favorable reduction route of CO2 to methanol was as follows: CO2 -> COOH* -> CO*+H2O -> CHO* -> CH2O* -> CH2OH* -> CH3OH. The FE of electrochemical CO2 reduction to methanol over Cu@Cu2O-400 degrees C electrocatalyst was >= 35% at-0.6 similar to-1.0 V (vs. RHE). The Cu@Cu2O-400 degrees C electrocatalyst exhibited a peak FECH3OH of 45% at-0.7 V, which was attributed to synergistic effect between Cu-0 and Cu+ active sites.
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