Electrochemical CO2-to-ethylene conversion on metal-free covalent quinazoline network-derived electrodes

Xian Suo; Fengtao Zhang; Zhenzhen Yang; Lu Wang; Ming Lei; James A. Gaugler; Meijia Li; Juntian Fan; Bishnu P. Thapaliya; Ilja Popovs; Alexander S. Ivanov; Leighanne C. Gallington; De en Jiang; Zhimin Liu; Sheng Dai

doi:10.1016/j.checat.2023.100506

Electrochemical CO₂-to-ethylene conversion on metal-free covalent quinazoline network-derived electrodes

Xian Suo, Fengtao Zhang, Zhenzhen Yang, Lu Wang, Ming Lei, James A. Gaugler, Meijia Li, Juntian Fan, Bishnu P. Thapaliya, Ilja Popovs, Alexander S. Ivanov, Leighanne C. Gallington, De en Jiang, Zhimin Liu, Sheng Dai

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

3 Scopus citations

Abstract

Electrocatalytic CO₂ reduction to produce multi-carbon (C₂₊) chemicals represents a highly attractive route for CO₂ utilization, particularly CO₂-to-ethene conversion toward fuel generation from renewable resources. However, state-of-the-art electrocatalysts are mainly limited to Cu-derived electrodes. Herein, metal-free nanoporous and defect-abundant covalent quinazoline network (CQN)-derived electrocatalysts displayed promising catalytic efficiency and selectivity in CO₂-to-ethene conversion. The highest Faradaic efficiency of ethene production (FE_C2H4) achieved 61.1% at −1.07 V (versus reversible hydrogen electrode [RHE]) by modified CQN-derived electrodes, surpassing the current metal-free systems in CO₂-to-ethene conversion. Structural characterization and theoretical calculation underscored the critical role of defect creation and the periphery nitrogen species in the tricycloquinazoline (TCQ) units in CO₂ adsorption, hydrogenation, and subsequent C–C coupling reaction to afford ethene. The achievements made in this work provide an alternative platform of metal-free nanocatalysts toward CO₂-to-C₂₊ products via electroreduction by leveraging the highly porous, extensively conjugated, and aza-fused ring-abundant two-dimensional networks.

Original language	English
Article number	100506
Journal	Chem Catalysis
Volume	3
Issue number	2
DOIs	https://doi.org/10.1016/j.checat.2023.100506
State	Published - Feb 16 2023

Funding

The research was supported financially by the Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, US Department of Energy . Use of the Advanced Photon Source at Argonne National Laboratory was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, under contract no. DE-AC02-06CH11357 .

Funders	Funder number
U.S. Department of Energy
Office of Science	DE-AC02-06CH11357
Basic Energy Sciences
Chemical Sciences, Geosciences, and Biosciences Division

Keywords

CO chemistry
CO electroreduction
SDG7: Affordable and clean energy
covalent quinazoline networks
ethene
metal-free catalysis

UN SDGs

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

Access to Document

10.1016/j.checat.2023.100506

Cite this

Suo, X., Zhang, F., Yang, Z., Wang, L., Lei, M., Gaugler, J. A., Li, M., Fan, J., Thapaliya, B. P., Popovs, I., Ivanov, A. S., Gallington, L. C., Jiang, D. E., Liu, Z., & Dai, S. (2023). Electrochemical CO₂-to-ethylene conversion on metal-free covalent quinazoline network-derived electrodes. Chem Catalysis, 3(2), Article 100506. https://doi.org/10.1016/j.checat.2023.100506

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abstract = "Electrocatalytic CO2 reduction to produce multi-carbon (C2+) chemicals represents a highly attractive route for CO2 utilization, particularly CO2-to-ethene conversion toward fuel generation from renewable resources. However, state-of-the-art electrocatalysts are mainly limited to Cu-derived electrodes. Herein, metal-free nanoporous and defect-abundant covalent quinazoline network (CQN)-derived electrocatalysts displayed promising catalytic efficiency and selectivity in CO2-to-ethene conversion. The highest Faradaic efficiency of ethene production (FEC2H4) achieved 61.1% at −1.07 V (versus reversible hydrogen electrode [RHE]) by modified CQN-derived electrodes, surpassing the current metal-free systems in CO2-to-ethene conversion. Structural characterization and theoretical calculation underscored the critical role of defect creation and the periphery nitrogen species in the tricycloquinazoline (TCQ) units in CO2 adsorption, hydrogenation, and subsequent C–C coupling reaction to afford ethene. The achievements made in this work provide an alternative platform of metal-free nanocatalysts toward CO2-to-C2+ products via electroreduction by leveraging the highly porous, extensively conjugated, and aza-fused ring-abundant two-dimensional networks.",

keywords = "CO chemistry, CO electroreduction, SDG7: Affordable and clean energy, covalent quinazoline networks, ethene, metal-free catalysis",

author = "Xian Suo and Fengtao Zhang and Zhenzhen Yang and Lu Wang and Ming Lei and Gaugler, {James A.} and Meijia Li and Juntian Fan and Thapaliya, {Bishnu P.} and Ilja Popovs and Ivanov, {Alexander S.} and Gallington, {Leighanne C.} and Jiang, {De en} and Zhimin Liu and Sheng Dai",

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doi = "10.1016/j.checat.2023.100506",

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AU - Suo, Xian

AU - Zhang, Fengtao

AU - Yang, Zhenzhen

AU - Wang, Lu

AU - Lei, Ming

AU - Gaugler, James A.

AU - Li, Meijia

AU - Fan, Juntian

AU - Thapaliya, Bishnu P.

AU - Popovs, Ilja

AU - Ivanov, Alexander S.

AU - Gallington, Leighanne C.

AU - Jiang, De en

AU - Liu, Zhimin

AU - Dai, Sheng

PY - 2023/2/16

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AB - Electrocatalytic CO2 reduction to produce multi-carbon (C2+) chemicals represents a highly attractive route for CO2 utilization, particularly CO2-to-ethene conversion toward fuel generation from renewable resources. However, state-of-the-art electrocatalysts are mainly limited to Cu-derived electrodes. Herein, metal-free nanoporous and defect-abundant covalent quinazoline network (CQN)-derived electrocatalysts displayed promising catalytic efficiency and selectivity in CO2-to-ethene conversion. The highest Faradaic efficiency of ethene production (FEC2H4) achieved 61.1% at −1.07 V (versus reversible hydrogen electrode [RHE]) by modified CQN-derived electrodes, surpassing the current metal-free systems in CO2-to-ethene conversion. Structural characterization and theoretical calculation underscored the critical role of defect creation and the periphery nitrogen species in the tricycloquinazoline (TCQ) units in CO2 adsorption, hydrogenation, and subsequent C–C coupling reaction to afford ethene. The achievements made in this work provide an alternative platform of metal-free nanocatalysts toward CO2-to-C2+ products via electroreduction by leveraging the highly porous, extensively conjugated, and aza-fused ring-abundant two-dimensional networks.

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KW - SDG7: Affordable and clean energy

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