Mechanistic routes toward C₃ products in copper-catalysed CO₂ electroreduction

Abstract

The mechanistic insights of CO2 electrochemical reduction on Cu materials up to C3 fragments are investigated by combining experiments and theory.

Assessing the economic potential of large-scale carbonate-formation-free CO2 electrolysis

“…The electrochemical CO 2 reduction reaction (CO 2 RR) can utilize CO 2 by valorizing it into fuels and basic chemicals. 1,2 Recent advances in CO 2 electroreduction have been motivating academia and industry to look into the economic viability of this technology. Therefore, many TEA analyses were carried out to find the threshold for profitability.…”

Modeling Operando Electrochemical CO2 Reduction

“…Experimental and theoretical insights into C 3+ products are limited by the complexity of the reaction mechanism and the low selectivity of these products, which prevents spectroscopic observation of the potential intermediates and comprehensive screening of electrochemical reduction experiments for key reagents. Even though sequential CO trimerization has been proposed in the past, currently the expected coupling mechanism toward C 3 products involves a OC­(H)­CH 2 –C­(H)O precursor, , potentially involving allyl alcohol (CH 2 CHCH 2 OH) and propionaldehyde (CH 3 CH 2 CHO) at later reduction stages (Figure b) . In fact, FE toward propanol, allyl alcohol, and propionaldehyde for eCO 2 R exhibits similar dependencies on applied potential for a polycrystalline copper catalysts and were equally promoted on Ag-decorated Cu 2 O nanocubes As for C 4 products, to date, two main reaction pathways have been proposed for the formation of 1-butanol, the only species observed at significant rate. , Both reaction schemes highlight the key role of an acetaldehyde precursor.…”

“…Experimental and theoretical insights into C 3+ products are limited by the complexity of the reaction mechanism and the low selectivity of these products, which prevents spectroscopic observation of the potential intermediates and comprehensive 15b). 334 In fact, FE toward propanol, allyl alcohol, and propionaldehyde for eCO 2 R exhibits similar dependencies on applied potential for a polycrystalline copper catalysts 106 and were equally promoted on Ag-decorated Cu 2 O nanocubes 154 As for C 4 products, to date, two main reaction pathways have been proposed for the formation of 1butanol, the only species observed at significant rate. 94,338 Both reaction schemes highlight the key role of an acetaldehyde precursor.…”

“…eCO 2 R pathway toward major (a) C 1 and (b), C 2+ products on metals. Experimental observations are taken from refs and . The CO–CO dimer bound to a near-surface oxygen is the deprotonated glyoxylate geometry predicted on OD–Cu. , n is equal to 3 and 1 for reduction of glyoxal (OCHOCH) and glycolaldehyde (HOCH 2 CHO) to *OCHCH 2 .…”

“…of electrochemical reduction experiments for key reagents. Even though sequential CO trimerization has been proposed in the past,337 currently the expected coupling mechanism toward C 3 products involves a OC(H)CH 2 −C(H) O precursor,156,334 potentially involving allyl alcohol (CH 2 CHCH 2 OH) and propionaldehyde (CH 3 CH 2 CHO) at later reduction stages (Figure…”