Dataset Information

Click-Derived Triazoles and Triazolylidenes of Manganese for Electrocatalytic Reduction of CO2.

ABSTRACT: A series of new fac-[Mn(L)(CO)3Br] complexes where L is a bidentate chelating ligand containing mixed mesoionic triazolylidene-pyridine (MIC^py, 1), triazolylidene-triazole (MIC^trz, 2), and triazole-pyridine (trz^py, 3) ligands have been prepared and fully characterized, including the single crystal X-ray diffraction studies of 1 and 2. The abilities of 1-3 and complex fac-[Mn(MIC^MIC)(CO)3Br] (4) to catalyze the electroreduction of CO2 has been assessed for the first time. It was found that all complexes displayed a current increase under CO2 atmosphere, being 3 and 4 the most active complexes. Complex 3, bearing a N^N-based ligand exhibited a good efficiency and an excellent selectivity for reducing CO2 to CO in the presence of 1.0 M of water, at low overpotential. Interestingly, complex 4 containing the strongly electron donating di-imidazolylidene ligand exhibited comparable activity to 3, when the experiments were performed in neat acetonitrile at slightly higher overpotential (-1.86 vs. -2.14 V).

SUBMITTER: Friaes S

PROVIDER: S-EPMC8588546 | biostudies-literature | 2021 Oct

REPOSITORIES: biostudies-literature

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Click-Derived Triazoles and Triazolylidenes of Manganese for Electrocatalytic Reduction of CO2.

Friães Sofia S Realista Sara S Gomes Clara S B CSB Martinho Paulo N PN Royo Beatriz B

Molecules (Basel, Switzerland) 20211020 21

A series of new fac-[Mn(L)(CO)3Br] complexes where L is a bidentate chelating ligand containing mixed mesoionic triazolylidene-pyridine (MIC^py, 1), triazolylidene-triazole (MIC^trz, 2), and triazole-pyridine (trz^py, 3) ligands have been prepared and fully characterized, including the single crystal X-ray diffraction studies of 1 and 2. The abilities of 1-3 and complex fac-[Mn(MIC^MIC)(CO)3Br] (4) to cat ...[more]

PMID: 34770734

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Project description:Abstract It remains a real challenge to control the selectivity of the electrocatalytic CO2 reduction (eCO2R) reaction to valuable chemicals and fuels. Most of the electrocatalysts are made of non‐renewable metal resources, which hampers their large‐scale implementation. Here, we report the preparation of bimetallic copper‐lead (CuPb) electrocatalysts from industrial metallurgical waste. The metal ions were extracted from the metallurgical waste through simple chemical treatment with ammonium chloride, and CuxPby electrocatalysts with tunable compositions were fabricated through electrodeposition at varying cathodic potentials. X‐ray spectroscopy techniques showed that the pristine electrocatalysts consist of Cu0, Cu1+ and Pb2+ domains, and no evidence for alloy formation was found. We found a volcano‐shape relationship between eCO2R selectivity toward two electron products, such as CO, and the elemental ratio of Cu and Pb. A maximum Faradaic efficiency towards CO was found for Cu9.00Pb1.00, which was four times higher than that of pure Cu, under the same electrocatalytic conditions. In situ Raman spectroscopy revealed that the optimal amount of Pb effectively improved the reducibility of the pristine Cu1+ and Pb2+ domains to metallic Cu and Pb, which boosted the selectivity towards CO by synergistic effects. This work provides a framework of thinking to design and tune the selectivity of bimetallic electrocatalysts for CO2 reduction through valorization of metallurgical waste. Bimetallic Cu‐Pb electrocatalysts were prepared from industrial metallurgical residues and used to electrochemically convert CO2 into valuable chemicals. The metlas were extracted through chemical treatment with ammonium chloride, and Cu−Pb electrocatalysts with varying ratios were prepared through electrodeposition. Compared with pure Cu, the bimetallic catalyst displayed a promotional effect on the conversion of carbon dioxide to carbon monoxide. In situ and ex situ characterization revealed that the interplay between in situ reduced Cu and Pb sites results in boosted CO production through synergistic effects.

Dataset Information

Click-Derived Triazoles and Triazolylidenes of Manganese for Electrocatalytic Reduction of CO2.

Publications

Click-Derived Triazoles and Triazolylidenes of Manganese for Electrocatalytic Reduction of CO<sub>2</sub>.

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