Acetic acid is an important chemical feedstock. The electrocatalytic synthesis of acetic acid from CO2 offers a low-carbon alternative to traditional synthetic routes, but the direct reduction from CO2 comes with a CO2 crossover energy penalty. CO electroreduction bypasses this, which motivates the interest in a cascade synthesis approach of CO2 to CO followed by CO to acetic acid. Here we report a catalyst design strategy in which off-target intermediates (such as ethylene and ethanol) in the reduction of CO to acetate are destabilized. On the optimized Ag–CuO2 catalyst, this destabilization of off-target intermediates leads to an acetate Faradaic efficiency of 70% at 200 mA cm−2. We demonstrate 18 hours of stable operation in a membrane electrode assembly; the system produced 5 wt% acetate at 100 mA cm−2 and a full-cell energy efficiency of 25%, a twofold improvement on the highest energy-efficient electrosynthesis in prior reports.
A silver–copper oxide catalyst for acetate electrosynthesis from carbon monoxide / R. Dorakhan, I. Grigioni, B. Lee, P. Ou, J. Abed, C. O’Brien, A. Sedighian Rasouli, M. Plodinec, R.K. Miao, E. Shirzadi, J. Wicks, S. Park, G. Lee, J. Zhang, D. Sinton, E.H. Sargent. - In: NATURE SYNTHESIS. - ISSN 2731-0582. - 2:5(2023), pp. 448-457. [10.1038/s44160-023-00259-w]
A silver–copper oxide catalyst for acetate electrosynthesis from carbon monoxide
I. GrigioniCo-primo
;
2023
Abstract
Acetic acid is an important chemical feedstock. The electrocatalytic synthesis of acetic acid from CO2 offers a low-carbon alternative to traditional synthetic routes, but the direct reduction from CO2 comes with a CO2 crossover energy penalty. CO electroreduction bypasses this, which motivates the interest in a cascade synthesis approach of CO2 to CO followed by CO to acetic acid. Here we report a catalyst design strategy in which off-target intermediates (such as ethylene and ethanol) in the reduction of CO to acetate are destabilized. On the optimized Ag–CuO2 catalyst, this destabilization of off-target intermediates leads to an acetate Faradaic efficiency of 70% at 200 mA cm−2. We demonstrate 18 hours of stable operation in a membrane electrode assembly; the system produced 5 wt% acetate at 100 mA cm−2 and a full-cell energy efficiency of 25%, a twofold improvement on the highest energy-efficient electrosynthesis in prior reports.File | Dimensione | Formato | |
---|---|---|---|
Manuscript__NATSYNTH.pdf
accesso aperto
Descrizione: Ultima versione inviata all'editor durante la fase di revisione
Tipologia:
Pre-print (manoscritto inviato all'editore)
Dimensione
1.24 MB
Formato
Adobe PDF
|
1.24 MB | Adobe PDF | Visualizza/Apri |
s44160-023-00259-w.pdf
accesso riservato
Descrizione: Article
Tipologia:
Publisher's version/PDF
Dimensione
2.68 MB
Formato
Adobe PDF
|
2.68 MB | Adobe PDF | Visualizza/Apri Richiedi una copia |
Pubblicazioni consigliate
I documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.