Electrolysis of ethylene to ethylene glycol paired with acidic CO2-to-CO conversion

Hongjun Chen; Heejong Shin; Jianan Erick Huang; Hengzhou Liu; Rui Kai Miao; Rong Xia; Weiyan Ni; Jiaqi Yu; Yongxiang Liang; Bosi Peng; Yuanjun Chen; Guangcan Su; Ke Xie; Anita Ho-Baillie; Edward H. Sargent

doi:10.1039/D5EE02847G

Electrolysis of ethylene to ethylene glycol paired with acidic CO₂-to-CO conversion

Hongjun Chen,†*^abd Heejong Shin,†‡^cd Jianan Erick Huang,†^cd Hengzhou Liu,

^cd Rui Kai Miao,^e Rong Xia,^cd Weiyan Ni,^cd Jiaqi Yu,^cd Yongxiang Liang,^cd Bosi Peng,^cd Yuanjun Chen,^cd Guangcan Su,

^cd Ke Xie,*^cd Anita Ho-Baillie

*^ab and Edward H. Sargent

*^cd

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* Corresponding authors

^a School of Physics, Faculty of Science, The University of Sydney, Sydney, NSW 2006, Australia
E-mail: hongjun.chen@sydney.edu.au, anita.ho-baillie@sydney.edu.au

^b The University of Sydney Nano Institute, The University of Sydney, Sydney, NSW 2006, Australia

^c Department of Chemistry, Northwestern University, Evanston, Illinois, USA
E-mail: ke-xie@northwestern.edu, ted.sargent@northwestern.edu

^d Department of Electrical and Computer Engineering, Northwestern University, Evanston, Illinois, USA

^e Department of Mechanical and Industrial Engineering, University of Toronto, Toronto, Ontario, Canada

Abstract

Electrochemical conversion of CO₂ into CO, ethylene, and other valuable chemicals is a promising method for carbon capture and utilisation. However, when carried out in an alkaline or neutral media, (bi)carbonate formation leads to low atom efficiency in the electrocatalytic process. In contrast, acidic conditions enable >80% CO₂ utilization, but there is a need to lower full-cell voltage. In this work, we paired the acidic cathodic CO₂-to-CO reaction with acidic anodic ethylene-to-ethylene glycol (C₂H₄-to-EG) conversion for the first time. For the selective oxidation of ethylene to EG, we employed a homogeneous redox mediator ruthenium–polyoxometalate (Ru–POM) with gold-modified electrodes for the first time to facilitate the redox cycle. This resulted in enhanced selectivity and stability, achieving a faradaic efficiency (FE) of 83% for EG. At the cathode, a porous nickel single-atom catalyst drives the conversion of CO₂ into CO in an acidic electrolyte with an FE of 97%. The paired system operates at a full-cell voltage of 3.1 V, compared to 3.3 V for a reference system using the oxygen evolution reaction. The demonstrated system offers a promising route for reducing carbon emissions with high atom efficiency.

Energy & Environmental Science

Electrolysis of ethylene to ethylene glycol paired with acidic CO₂-to-CO conversion

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Electrolysis of ethylene to ethylene glycol paired with acidic CO₂-to-CO conversion

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