Zhao, Q;
Lei, K;
Xia, BY;
Crespo-Otero, R;
Di Tommaso, D;
(2024)
Molecular engineering binuclear copper catalysts for selective CO<inf>2</inf> reduction to C<inf>2</inf> products.
Journal of Energy Chemistry
, 93
pp. 166-173.
10.1016/j.jechem.2024.01.060.
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Abstract
Molecular copper catalysts serve as exemplary models for correlating the structure-reaction-mechanism relationship in the electrochemical CO2 reduction (eCO2R), owing to their adaptable environments surrounding the copper metal centres. This investigation, employing density functional theory calculations, focuses on a novel family of binuclear Cu molecular catalysts. The modulation of their coordination configuration through the introduction of organic groups aims to assess their efficacy in converting CO2 to C2 products. Our findings highlight the crucial role of chemical valence state in shaping the characteristics of binuclear Cu catalysts, consequently influencing the eCO2R behaviour. Notably, the Cu(II)Cu(II) macrocycle catalyst exhibits enhanced suppression of the hydrogen evolution reaction (HER), facilitating proton transfer and the eCO2R process. Furthermore, we explore the impact of diverse electron-withdrawing and electron-donating groups coordinated to the macrocycle (R = –F, –H, and –OCH3) on the electron distribution in the molecular catalysts. Strategic placement of –OCH3 groups in the macrocycles leads to a favourable oxidation state of the Cu centres and subsequent C–C coupling to form C2 products. This research provides fundamental insights into the design and optimization of binuclear Cu molecular catalysts for the electrochemical conversion of CO2 to value-added C2 products.
| Type: | Article |
|---|---|
| Title: | Molecular engineering binuclear copper catalysts for selective CO<inf>2</inf> reduction to C<inf>2</inf> products |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1016/j.jechem.2024.01.060 |
| Publisher version: | https://doi.org/10.1016/j.jechem.2024.01.060 |
| Language: | English |
| Additional information: | This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third-party material in this article are included in the Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ |
| Keywords: | Molecular catalyst design, Selective CO2 reduction, C2 products, Density functional theory calculations |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10189379 |
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