The electrochemical CO2 reduction reaction (CO2RR) has progressed but suffers an energy penalty from CO2 loss due to carbonate formation and crossover. Cascade CO2 to CO conversion followed by CO reduction addresses this issue, but the combined figures of carbon efficiency (CE), energy efficiency (EE), selectivity, and stability require improvement. We posited that increased CO availability near active catalytic sites could maintain selectivity even under CO-depleted conditions. Here, we present a heterojunction carbon reservoir catalyst (CRC) architecture that combines copper nanoparticles with porous carbon nanoparticles. The pyridinic and pyrrolic functionalities of CRC can absorb CO enabling high CE under CO-depleted conditions. With CRC catalyst, we achieve ethanol FE and CE of 50% and 93% (CE∗Faradaic efficiency [FE] = 47%) in flow cell at 200 mA cm−2, fully doubling the best prior CE∗FE to ethanol. In membrane electrode assembly (MEA) system, we show sustained efficiency over 85 h at 100 mA cm−2.
High carbon efficiency in CO-to-alcohol electroreduction using a CO reservoir / S. Park, I. Grigioni, T. Alkayyali, B.-. Lee, J. Kim, E. Shirzadi, R. Dorakhan, G. Lee, J. Abed, F. Bossola, E.D. Jung, Y. Liang, M.G. Lee, A. Shayesteh Zeraati, D. Kim, D. Sinton, E. Sargent. - In: JOULE. - ISSN 2542-4351. - 7:10(2023), pp. 2335-2348. [10.1016/j.joule.2023.08.001]
High carbon efficiency in CO-to-alcohol electroreduction using a CO reservoir
I. GrigioniCo-primo
;
2023
Abstract
The electrochemical CO2 reduction reaction (CO2RR) has progressed but suffers an energy penalty from CO2 loss due to carbonate formation and crossover. Cascade CO2 to CO conversion followed by CO reduction addresses this issue, but the combined figures of carbon efficiency (CE), energy efficiency (EE), selectivity, and stability require improvement. We posited that increased CO availability near active catalytic sites could maintain selectivity even under CO-depleted conditions. Here, we present a heterojunction carbon reservoir catalyst (CRC) architecture that combines copper nanoparticles with porous carbon nanoparticles. The pyridinic and pyrrolic functionalities of CRC can absorb CO enabling high CE under CO-depleted conditions. With CRC catalyst, we achieve ethanol FE and CE of 50% and 93% (CE∗Faradaic efficiency [FE] = 47%) in flow cell at 200 mA cm−2, fully doubling the best prior CE∗FE to ethanol. In membrane electrode assembly (MEA) system, we show sustained efficiency over 85 h at 100 mA cm−2.File | Dimensione | Formato | |
---|---|---|---|
CarbonReservoirCatalyst_MS_Revised.pdf
Open Access dal 26/08/2024
Descrizione: Article
Tipologia:
Post-print, accepted manuscript ecc. (versione accettata dall'editore)
Dimensione
1.27 MB
Formato
Adobe PDF
|
1.27 MB | Adobe PDF | Visualizza/Apri |
Pubblicazioni consigliate
I documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.