Electrosynthesis of CO from an electrically pH-shifted DAC post-capture liquid using a catalyst:support amide linkage

Bei Zhou; Hengzhou Liu; Guangcan Su; Heejong Shin; Xiao Yan Li; Huajie Ze; Yongxiang Liang; Bosi Peng; Weiyan Ni; Yuanjun Chen; Wenjin Zhu; Christine Yu; Yiqing Chen; Pengfei Ou; Ke Xie; Edward H. Sargent

doi:10.1016/j.joule.2025.101883

Electrosynthesis of CO from an electrically pH-shifted DAC post-capture liquid using a catalyst:support amide linkage

Bei Zhou, Hengzhou Liu, Guangcan Su, Heejong Shin, Xiao Yan Li, Huajie Ze, Yongxiang Liang, Bosi Peng, Weiyan Ni, Yuanjun Chen, Wenjin Zhu, Christine Yu, Yiqing Chen, Pengfei Ou, Ke Xie^*, Edward H. Sargent^*

^*Corresponding author for this work

Chemistry

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

Abstract

Electrified reactive capture upgrades CO₂ from post-air-capture alkali carbonate liquid to value-added products while regenerating the capture medium. Previous processes exhibited limited energy efficiency (<18%) due to high full-cell voltage (>3.7 V) and modest CO selectivity (<45%). To address this, we developed a Co molecular catalyst featuring an electron-deficient Co center, lowering the required reduction voltage. We then grafted the catalyst onto a conductive support, enhancing charge transfer. An electrified pH-downshifter improved CO₂ availability, increasing CO selectivity. The system achieved 70% CO selectivity at 2.7 V and 100 mA cm⁻², corresponding to an energy intensity of 35 GJ/ton CO. The energy cost is comparable to that of direct air capture (DAC) followed by reverse water-gas shift (RWGS), but it offers ambient temperature operation.

Original language	English (US)
Article number	101883
Journal	Joule
Volume	9
Issue number	5
DOIs	https://doi.org/10.1016/j.joule.2025.101883
State	Published - May 21 2025

Funding

This work received support from Office of Naval Research under the agreement no. N00014-22-1-2690.

Keywords

CO conversion
bipolar membrane
closed loop
direct air capture
in situ CO utilization
integrated CO capture and utilization
support effect

ASJC Scopus subject areas

General Energy

UN SDGs

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

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10.1016/j.joule.2025.101883

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title = "Electrosynthesis of CO from an electrically pH-shifted DAC post-capture liquid using a catalyst:support amide linkage",

abstract = "Electrified reactive capture upgrades CO2 from post-air-capture alkali carbonate liquid to value-added products while regenerating the capture medium. Previous processes exhibited limited energy efficiency (<18%) due to high full-cell voltage (>3.7 V) and modest CO selectivity (<45%). To address this, we developed a Co molecular catalyst featuring an electron-deficient Co center, lowering the required reduction voltage. We then grafted the catalyst onto a conductive support, enhancing charge transfer. An electrified pH-downshifter improved CO2 availability, increasing CO selectivity. The system achieved 70% CO selectivity at 2.7 V and 100 mA cm−2, corresponding to an energy intensity of 35 GJ/ton CO. The energy cost is comparable to that of direct air capture (DAC) followed by reverse water-gas shift (RWGS), but it offers ambient temperature operation.",

keywords = "CO conversion, bipolar membrane, closed loop, direct air capture, in situ CO utilization, integrated CO capture and utilization, support effect",

author = "Bei Zhou and Hengzhou Liu and Guangcan Su and Heejong Shin and Li, {Xiao Yan} and Huajie Ze and Yongxiang Liang and Bosi Peng and Weiyan Ni and Yuanjun Chen and Wenjin Zhu and Christine Yu and Yiqing Chen and Pengfei Ou and Ke Xie and Sargent, {Edward H.}",

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year = "2025",

month = may,

day = "21",

doi = "10.1016/j.joule.2025.101883",

language = "English (US)",

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T1 - Electrosynthesis of CO from an electrically pH-shifted DAC post-capture liquid using a catalyst:support amide linkage

AU - Zhou, Bei

AU - Liu, Hengzhou

AU - Su, Guangcan

AU - Shin, Heejong

AU - Li, Xiao Yan

AU - Ze, Huajie

AU - Liang, Yongxiang

AU - Peng, Bosi

AU - Ni, Weiyan

AU - Chen, Yuanjun

AU - Zhu, Wenjin

AU - Yu, Christine

AU - Chen, Yiqing

AU - Ou, Pengfei

AU - Xie, Ke

AU - Sargent, Edward H.

PY - 2025/5/21

Y1 - 2025/5/21

N2 - Electrified reactive capture upgrades CO2 from post-air-capture alkali carbonate liquid to value-added products while regenerating the capture medium. Previous processes exhibited limited energy efficiency (<18%) due to high full-cell voltage (>3.7 V) and modest CO selectivity (<45%). To address this, we developed a Co molecular catalyst featuring an electron-deficient Co center, lowering the required reduction voltage. We then grafted the catalyst onto a conductive support, enhancing charge transfer. An electrified pH-downshifter improved CO2 availability, increasing CO selectivity. The system achieved 70% CO selectivity at 2.7 V and 100 mA cm−2, corresponding to an energy intensity of 35 GJ/ton CO. The energy cost is comparable to that of direct air capture (DAC) followed by reverse water-gas shift (RWGS), but it offers ambient temperature operation.

AB - Electrified reactive capture upgrades CO2 from post-air-capture alkali carbonate liquid to value-added products while regenerating the capture medium. Previous processes exhibited limited energy efficiency (<18%) due to high full-cell voltage (>3.7 V) and modest CO selectivity (<45%). To address this, we developed a Co molecular catalyst featuring an electron-deficient Co center, lowering the required reduction voltage. We then grafted the catalyst onto a conductive support, enhancing charge transfer. An electrified pH-downshifter improved CO2 availability, increasing CO selectivity. The system achieved 70% CO selectivity at 2.7 V and 100 mA cm−2, corresponding to an energy intensity of 35 GJ/ton CO. The energy cost is comparable to that of direct air capture (DAC) followed by reverse water-gas shift (RWGS), but it offers ambient temperature operation.

KW - CO conversion

KW - bipolar membrane

KW - closed loop

KW - direct air capture

KW - in situ CO utilization

KW - integrated CO capture and utilization

KW - support effect

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Electrosynthesis of CO from an electrically pH-shifted DAC post-capture liquid using a catalyst:support amide linkage

Abstract

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Keywords

ASJC Scopus subject areas

UN SDGs

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