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

doi:10.1016/j.joule.2023.08.001

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

Department of Chemistry & Nanoscience

Research output: Contribution to journal › Article › peer-review

5 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 language	English
Pages (from-to)	2335-2348
Number of pages	14
Journal	Joule
Volume	7
Issue number	10
DOIs	https://doi.org/10.1016/j.joule.2023.08.001
State	Published - 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

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1016/j.joule.2023.08.001

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title = "High carbon efficiency in CO-to-alcohol electroreduction using a CO reservoir",

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.",

keywords = "CO electroreduction, CO electroreduction, CO valorization, carbon monoxide, carbon utilization, electrocatalysis, ethanol, nitrogen-doped carbon, porosity control, renewable fuels",

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

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T1 - High carbon efficiency in CO-to-alcohol electroreduction using a CO reservoir

AU - Park, Sungjin

AU - Grigioni, Ivan

AU - Alkayyali, Tartela

AU - Lee, Byoung Hoon

AU - Kim, Jiheon

AU - Shirzadi, Erfan

AU - Dorakhan, Roham

AU - Lee, Geonhui

AU - Abed, Jehad

AU - Bossola, Filippo

AU - Jung, Eui Dae

AU - Liang, Yongxiang

AU - Lee, Mi Gyoung

AU - Shayesteh Zeraati, Ali

AU - Kim, Dongha

AU - Sinton, David

AU - Sargent, Edward

PY - 2023/10/18

Y1 - 2023/10/18

N2 - 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.

AB - 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.

KW - CO electroreduction

KW - CO valorization

KW - carbon monoxide

KW - carbon utilization

KW - electrocatalysis

KW - ethanol

KW - nitrogen-doped carbon

KW - porosity control

KW - renewable fuels

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

Abstract

Bibliographical note

Keywords

UN SDGs

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