High carbon efficiency in CO-to-alcohol electroreduction using a CO reservoir

Sungjin Park, Ivan Grigioni, Tartela Alkayyali, Byoung Hoon Lee, Jiheon Kim, Erfan Shirzadi, Roham Dorakhan, Geonhui Lee, Jehad Abed, Filippo Bossola, Eui Dae Jung, Yongxiang Liang, Mi Gyoung Lee, Ali Shayesteh Zeraati, Dongha Kim, David Sinton, Edward Sargent

Research output: Contribution to journalArticlepeer-review

3 Scopus citations

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.

Original languageEnglish
Pages (from-to)2335-2348
Number of pages14
JournalJoule
Volume7
Issue number10
DOIs
StatePublished - 18 Oct 2023

Bibliographical note

Publisher Copyright:
© 2023 Elsevier Inc.

Keywords

  • CO electroreduction
  • CO electroreduction
  • CO valorization
  • carbon monoxide
  • carbon utilization
  • electrocatalysis
  • ethanol
  • nitrogen-doped carbon
  • porosity control
  • renewable fuels

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