Back to Search
Start Over
Lewis-Basic EDTA as a Highly Active Molecular Electrocatalyst for CO 2 Reduction to CH 4 .
- Source :
-
Angewandte Chemie (International ed. in English) [Angew Chem Int Ed Engl] 2021 Oct 11; Vol. 60 (42), pp. 23002-23009. Date of Electronic Publication: 2021 Sep 12. - Publication Year :
- 2021
-
Abstract
- The most active catalysts so far successful in hydrogenation reduction of CO <subscript>2</subscript> are mainly heterogeneous Cu-based catalysts. The complex coordination environments and multiple active sites in heterogeneous catalysts result in low selectivity of target product, while molecular catalysts with well-defined active sites and tailorable structures allow mechanism-based performance optimization. Herein, we firstly report a single ethylenediaminetetraacetic acid (EDTA) molecular-level immobilized on the surface of carbon nanotube as a catalyst for transferring CO <subscript>2</subscript> to CH <subscript>4</subscript> with an excellent performance. This catalyst exhibits a high Faradaic efficiency of 61.6 % toward CH <subscript>4</subscript> , a partial current density of -16.5 mA cm <superscript>-2</superscript> at a potential of -1.3 V versus reversible hydrogen electrode. Density functional theory calculations reveal that the Lewis basic COO <superscript>-</superscript> groups in EDTA molecule are the active sites for CO <subscript>2</subscript> reduction reaction (CO <subscript>2</subscript> RR). The energy barrier for the generation of CO from *CO intermediate is as high as 0.52 eV, while the further protonation of *CO to *CHO follows an energetic downhill path (-1.57 eV), resulting in the high selectivity of CH <subscript>4</subscript> . This work makes it possible to control the product selectivity for CO <subscript>2</subscript> RR according to the relationship between the energy barrier of *CO intermediate and molecular structures in the future.<br /> (© 2021 Wiley-VCH GmbH.)
Details
- Language :
- English
- ISSN :
- 1521-3773
- Volume :
- 60
- Issue :
- 42
- Database :
- MEDLINE
- Journal :
- Angewandte Chemie (International ed. in English)
- Publication Type :
- Academic Journal
- Accession number :
- 34427034
- Full Text :
- https://doi.org/10.1002/anie.202110594