Functionalization of Carbon Nanotubes with Nickel Cyclam for the Electrochemical Reduction of CO2

Silvia Pugliese; Ngoc Tran Huan; Jérémy Forte; Domenico Grammatico; Sandrine Zanna; Bao Lian Su; Yun Li; Marc Fontecave

doi:10.1002/cssc.202002092

Functionalization of Carbon Nanotubes with Nickel Cyclam for the Electrochemical Reduction of CO₂

Silvia Pugliese, Ngoc Tran Huan, Jérémy Forte, Domenico Grammatico, Sandrine Zanna, Bao Lian Su, Yun Li, Marc Fontecave

University of Namur

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

Abstract

The exploitation of molecular catalysts for CO₂ electrolysis requires their immobilization on the cathode of the electrolyzer. As an illustration of this approach, a Ni-cyclam complex with a cyclam derivative functionalized with a pyrene moiety is synthesized, found to be a selective catalyst for CO₂ electroreduction to CO, and immobilized on a carbon nanotube-coated gas diffusion electrode by using a noncovalent binding strategy. The as-prepared electrode is efficient, selective, and robust for electrocatalytic reduction of CO₂ to CO. Very high turnover numbers (ca. 61460) and turnover frequencies (ca. 4.27 s⁻¹) are enabled by the novel electrode material in organic solvent-water mixtures saturated with CO₂. This material provides an interesting platform for further improvement.

Original language	English
Pages (from-to)	6449-6456
Number of pages	8
Journal	ChemSusChem
Volume	13
Issue number	23
Early online date	21 Oct 2020
DOIs	https://doi.org/10.1002/cssc.202002092
Publication status	Published - 7 Dec 2020

Keywords

carbon nanotubes
CO conversion
electrocatalysis
heterogenization
nickel Cyclam

UN SDGs

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

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10.1002/cssc.202002092

Cite this

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title = "Functionalization of Carbon Nanotubes with Nickel Cyclam for the Electrochemical Reduction of CO2",

abstract = "The exploitation of molecular catalysts for CO2 electrolysis requires their immobilization on the cathode of the electrolyzer. As an illustration of this approach, a Ni-cyclam complex with a cyclam derivative functionalized with a pyrene moiety is synthesized, found to be a selective catalyst for CO2 electroreduction to CO, and immobilized on a carbon nanotube-coated gas diffusion electrode by using a noncovalent binding strategy. The as-prepared electrode is efficient, selective, and robust for electrocatalytic reduction of CO2 to CO. Very high turnover numbers (ca. 61460) and turnover frequencies (ca. 4.27 s−1) are enabled by the novel electrode material in organic solvent-water mixtures saturated with CO2. This material provides an interesting platform for further improvement.",

keywords = "carbon nanotubes, CO conversion, electrocatalysis, heterogenization, nickel Cyclam",

author = "Silvia Pugliese and Huan, {Ngoc Tran} and J{\'e}r{\'e}my Forte and Domenico Grammatico and Sandrine Zanna and Su, {Bao Lian} and Yun Li and Marc Fontecave",

note = "Funding Information: S.P. and D.G. acknowledge financial support from the European School on Artificial Leaf: Electrodes & Devices (eSCALED). This project has received funding from the European's Union's Horizon 2020 research and innovation program under the Marie Sklodowska-Curie grant agreement No 765376. We thank Geoffrey Gontard (Sorbonne Universit{\'e}s) for solving the structure of cis-1 (DMF). We thank Francoise Pillier (Sorbonne Universit{\'e}s) for the SEM images. Funding Information: S.P. and D.G. acknowledge financial support from the European School on Artificial Leaf: Electrodes & Devices (eSCALED). This project has received funding from the European's Union's Horizon 2020 research and innovation program under the Marie Sklodowska‐Curie grant agreement No 765376. We thank Geoffrey Gontard (Sorbonne Universit{\'e}s) for solving the structure of cis‐ (DMF). We thank Francoise Pillier (Sorbonne Universit{\'e}s) for the SEM images. 1 Publisher Copyright: {\textcopyright} 2020 Wiley-VCH GmbH",

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doi = "10.1002/cssc.202002092",

language = "English",

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AU - Pugliese, Silvia

AU - Huan, Ngoc Tran

AU - Forte, Jérémy

AU - Grammatico, Domenico

AU - Zanna, Sandrine

AU - Su, Bao Lian

AU - Li, Yun

AU - Fontecave, Marc

N1 - Funding Information: S.P. and D.G. acknowledge financial support from the European School on Artificial Leaf: Electrodes & Devices (eSCALED). This project has received funding from the European's Union's Horizon 2020 research and innovation program under the Marie Sklodowska-Curie grant agreement No 765376. We thank Geoffrey Gontard (Sorbonne Universités) for solving the structure of cis-1 (DMF). We thank Francoise Pillier (Sorbonne Universités) for the SEM images. Funding Information: S.P. and D.G. acknowledge financial support from the European School on Artificial Leaf: Electrodes & Devices (eSCALED). This project has received funding from the European's Union's Horizon 2020 research and innovation program under the Marie Sklodowska‐Curie grant agreement No 765376. We thank Geoffrey Gontard (Sorbonne Universités) for solving the structure of cis‐ (DMF). We thank Francoise Pillier (Sorbonne Universités) for the SEM images. 1 Publisher Copyright: © 2020 Wiley-VCH GmbH

PY - 2020/12/7

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N2 - The exploitation of molecular catalysts for CO2 electrolysis requires their immobilization on the cathode of the electrolyzer. As an illustration of this approach, a Ni-cyclam complex with a cyclam derivative functionalized with a pyrene moiety is synthesized, found to be a selective catalyst for CO2 electroreduction to CO, and immobilized on a carbon nanotube-coated gas diffusion electrode by using a noncovalent binding strategy. The as-prepared electrode is efficient, selective, and robust for electrocatalytic reduction of CO2 to CO. Very high turnover numbers (ca. 61460) and turnover frequencies (ca. 4.27 s−1) are enabled by the novel electrode material in organic solvent-water mixtures saturated with CO2. This material provides an interesting platform for further improvement.

AB - The exploitation of molecular catalysts for CO2 electrolysis requires their immobilization on the cathode of the electrolyzer. As an illustration of this approach, a Ni-cyclam complex with a cyclam derivative functionalized with a pyrene moiety is synthesized, found to be a selective catalyst for CO2 electroreduction to CO, and immobilized on a carbon nanotube-coated gas diffusion electrode by using a noncovalent binding strategy. The as-prepared electrode is efficient, selective, and robust for electrocatalytic reduction of CO2 to CO. Very high turnover numbers (ca. 61460) and turnover frequencies (ca. 4.27 s−1) are enabled by the novel electrode material in organic solvent-water mixtures saturated with CO2. This material provides an interesting platform for further improvement.

KW - carbon nanotubes

KW - CO conversion

KW - electrocatalysis

KW - heterogenization

KW - nickel Cyclam

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JO - ChemSusChem

JF - ChemSusChem

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ER -

Functionalization of Carbon Nanotubes with Nickel Cyclam for the Electrochemical Reduction of CO₂

Abstract

Keywords

UN SDGs

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Functionalization of Carbon Nanotubes with Nickel Cyclam for the Electrochemical Reduction of CO2

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Keywords

UN SDGs

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Functionalization of Carbon Nanotubes with Nickel Cyclam for the Electrochemical Reduction of CO₂