Surface-Modified Carbon Materials for CO2 Electroreduction

Francesco Mattarozzi; Marisol Tapia Rosales; Rim C.J. van de Poll; Emiel J.M. Hensen; Peter Ngene; Petra E. de Jongh

doi:10.1002/ejic.202300152

Surface-Modified Carbon Materials for CO₂ Electroreduction

Francesco Mattarozzi, Marisol Tapia Rosales, Rim C.J. van de Poll, Emiel J.M. Hensen, Peter Ngene, Petra E. de Jongh^*

^*Corresponding author for this work

Eindhoven University of Technology

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

Abstract

The electrochemical reduction of CO₂ to produce sustainable fuels and chemicals has attracted great attention in recent years. It is shown that surface-modified carbons catalyze the CO₂RR. This study reports a strategy to modify the surface of commercially available carbon materials by adding oxygen and nitrogen surface groups without modifying its graphitic structure. Clear differences in CO₂RR activity, selectivity and the turnover frequency between the surface-modified carbons were observed, and these differences were ascribed to the nature of the surface groups chemistry and the point of zero charge (PZC). The results show that nitrogen-containing surface groups are highly selective towards the formation of CO from the electroreduction of CO₂ in comparison with the oxygen-containing surface groups, and the carbon without surface groups. This demonstrates that the selectivity of carbon for CO₂RR can be rationally tuned by simply altering the surface chemistry via surface functionalization.

Original language	English
Article number	e202300152
Journal	European Journal of Inorganic Chemistry
Volume	26
Issue number	28
DOIs	https://doi.org/10.1002/ejic.202300152
Publication status	Published - 2 Oct 2023

Bibliographical note

Funding Information:
Francesco Mattarozzi was supported in collaboration with Shell Global Solutions International B. V. via the Advanced Research Center Chemical Building Blocks Consortium (ARC-CBBC). Marisol Tapia Rosales was supported by the NWO-EleReCet project, part of the Solar-to-Products program funded by the Dutch Research Council (NWO). Jan Willem de Rijk is acknowledged for useful discussions on the electrochemical set-up. Iris ten Have is acknowledged for the SEM images.

Funding Information:
Francesco Mattarozzi was supported in collaboration with Shell Global Solutions International B. V. via the Advanced Research Center Chemical Building Blocks Consortium (ARC‐CBBC). Marisol Tapia Rosales was supported by the NWO‐EleReCet project, part of the Solar‐to‐Products program funded by the Dutch Research Council (NWO). Jan Willem de Rijk is acknowledged for useful discussions on the electrochemical set‐up. Iris ten Have is acknowledged for the SEM images.

Publisher Copyright:
© 2023 The Authors. European Journal of Inorganic Chemistry published by Wiley-VCH GmbH.

Funding

Francesco Mattarozzi was supported in collaboration with Shell Global Solutions International B. V. via the Advanced Research Center Chemical Building Blocks Consortium (ARC-CBBC). Marisol Tapia Rosales was supported by the NWO-EleReCet project, part of the Solar-to-Products program funded by the Dutch Research Council (NWO). Jan Willem de Rijk is acknowledged for useful discussions on the electrochemical set-up. Iris ten Have is acknowledged for the SEM images. Francesco Mattarozzi was supported in collaboration with Shell Global Solutions International B. V. via the Advanced Research Center Chemical Building Blocks Consortium (ARC‐CBBC). Marisol Tapia Rosales was supported by the NWO‐EleReCet project, part of the Solar‐to‐Products program funded by the Dutch Research Council (NWO). Jan Willem de Rijk is acknowledged for useful discussions on the electrochemical set‐up. Iris ten Have is acknowledged for the SEM images.

Keywords

Carbon materials
CO reduction reaction
electrochemistry
surface chemistry
surface modification

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10.1002/ejic.202300152Licence: CC BY

Eur J Inorg Chem - 2023 - Mattarozzi - Surface‐Modified Carbon Materials for CO2 ElectroreductionFinal published version, 1.1 MBLicence: CC BY

Cite this

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title = "Surface-Modified Carbon Materials for CO2 Electroreduction",

abstract = "The electrochemical reduction of CO2 to produce sustainable fuels and chemicals has attracted great attention in recent years. It is shown that surface-modified carbons catalyze the CO2RR. This study reports a strategy to modify the surface of commercially available carbon materials by adding oxygen and nitrogen surface groups without modifying its graphitic structure. Clear differences in CO2RR activity, selectivity and the turnover frequency between the surface-modified carbons were observed, and these differences were ascribed to the nature of the surface groups chemistry and the point of zero charge (PZC). The results show that nitrogen-containing surface groups are highly selective towards the formation of CO from the electroreduction of CO2 in comparison with the oxygen-containing surface groups, and the carbon without surface groups. This demonstrates that the selectivity of carbon for CO2RR can be rationally tuned by simply altering the surface chemistry via surface functionalization.",

keywords = "Carbon materials, CO reduction reaction, electrochemistry, surface chemistry, surface modification",

author = "Francesco Mattarozzi and {Tapia Rosales}, Marisol and {van de Poll}, {Rim C.J.} and Hensen, {Emiel J.M.} and Peter Ngene and {de Jongh}, {Petra E.}",

note = "Funding Information: Francesco Mattarozzi was supported in collaboration with Shell Global Solutions International B. V. via the Advanced Research Center Chemical Building Blocks Consortium (ARC-CBBC). Marisol Tapia Rosales was supported by the NWO-EleReCet project, part of the Solar-to-Products program funded by the Dutch Research Council (NWO). Jan Willem de Rijk is acknowledged for useful discussions on the electrochemical set-up. Iris ten Have is acknowledged for the SEM images. Funding Information: Francesco Mattarozzi was supported in collaboration with Shell Global Solutions International B. V. via the Advanced Research Center Chemical Building Blocks Consortium (ARC‐CBBC). Marisol Tapia Rosales was supported by the NWO‐EleReCet project, part of the Solar‐to‐Products program funded by the Dutch Research Council (NWO). Jan Willem de Rijk is acknowledged for useful discussions on the electrochemical set‐up. Iris ten Have is acknowledged for the SEM images. Publisher Copyright: {\textcopyright} 2023 The Authors. European Journal of Inorganic Chemistry published by Wiley-VCH GmbH.",

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AU - van de Poll, Rim C.J.

AU - Hensen, Emiel J.M.

AU - Ngene, Peter

AU - de Jongh, Petra E.

N1 - Funding Information: Francesco Mattarozzi was supported in collaboration with Shell Global Solutions International B. V. via the Advanced Research Center Chemical Building Blocks Consortium (ARC-CBBC). Marisol Tapia Rosales was supported by the NWO-EleReCet project, part of the Solar-to-Products program funded by the Dutch Research Council (NWO). Jan Willem de Rijk is acknowledged for useful discussions on the electrochemical set-up. Iris ten Have is acknowledged for the SEM images. Funding Information: Francesco Mattarozzi was supported in collaboration with Shell Global Solutions International B. V. via the Advanced Research Center Chemical Building Blocks Consortium (ARC‐CBBC). Marisol Tapia Rosales was supported by the NWO‐EleReCet project, part of the Solar‐to‐Products program funded by the Dutch Research Council (NWO). Jan Willem de Rijk is acknowledged for useful discussions on the electrochemical set‐up. Iris ten Have is acknowledged for the SEM images. Publisher Copyright: © 2023 The Authors. European Journal of Inorganic Chemistry published by Wiley-VCH GmbH.

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N2 - The electrochemical reduction of CO2 to produce sustainable fuels and chemicals has attracted great attention in recent years. It is shown that surface-modified carbons catalyze the CO2RR. This study reports a strategy to modify the surface of commercially available carbon materials by adding oxygen and nitrogen surface groups without modifying its graphitic structure. Clear differences in CO2RR activity, selectivity and the turnover frequency between the surface-modified carbons were observed, and these differences were ascribed to the nature of the surface groups chemistry and the point of zero charge (PZC). The results show that nitrogen-containing surface groups are highly selective towards the formation of CO from the electroreduction of CO2 in comparison with the oxygen-containing surface groups, and the carbon without surface groups. This demonstrates that the selectivity of carbon for CO2RR can be rationally tuned by simply altering the surface chemistry via surface functionalization.

AB - The electrochemical reduction of CO2 to produce sustainable fuels and chemicals has attracted great attention in recent years. It is shown that surface-modified carbons catalyze the CO2RR. This study reports a strategy to modify the surface of commercially available carbon materials by adding oxygen and nitrogen surface groups without modifying its graphitic structure. Clear differences in CO2RR activity, selectivity and the turnover frequency between the surface-modified carbons were observed, and these differences were ascribed to the nature of the surface groups chemistry and the point of zero charge (PZC). The results show that nitrogen-containing surface groups are highly selective towards the formation of CO from the electroreduction of CO2 in comparison with the oxygen-containing surface groups, and the carbon without surface groups. This demonstrates that the selectivity of carbon for CO2RR can be rationally tuned by simply altering the surface chemistry via surface functionalization.

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