Electrocatalytic properties of a novel ruthenium(<scp>ii</scp>) terpyridine-based complex towards CO<sub>2</sub> reduction

Faustino, Leandro A.; Machado, Antonio Liles Tavares; Maia, Pedro Ivo da Silva; Concepcion, Javier J.; Patrocínio, Antonio Otávio T.

doi:10.1039/d3dt00121k

Dalton Trans.

2023

DOI: 10.1039/d3dt00121k

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Electrocatalytic properties of a novel ruthenium(ii) terpyridine-based complex towards CO₂ reduction

Leandro A. Faustino

Antonio Liles Tavares Machado

Pedro Ivo da Silva Maia³

et al.

Abstract: The electrocatalytic properties of Ru complexes are of great technological interest given their potential application in reactions such water splitting and CO2 reduction. In this work, a novel terpyridine-based Ru(II)...

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Diiron Complexes with Rigid and Conjugated S-to-S Bridges for Electrocatalytic Reduction of CO₂

Cheng,

Shen,

Zhang

et al. 2024

Inorg. Chem.

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Electroreduction of CO2 to value-added low-carbon chemicals is a promising way for carbon neutrality and CO2 utilization. It was found that the diiron complex [(μ-bdt)Fe2(CO)6] (bdt = benzene-1,2-dithiolate) has high catalytic activity for electrocatalytic CO2 reduction. To further study the effect of the S-to-S bridge on the catalytic performances of diiron complexes for electrochemical CO2 reduction, four diiron complexes 1–4 with different rigid and conjugated S-to-S bridges were either selected or designed. The electrocatalytic studies showed that under optimal conditions, 2 with a 2,3-naphthalenedithiolato bridge exhibited the lowest catalytic onset potential (E onset = −1.75 V vs Fc+/0), while 4 with a diphenyl-1,2-vinylidene bridge displayed the highest catalytic activity (TOFmax = 295 s–1), which is 1.5 times that of [(μ-bdt)Fe2(CO)6]. The controlled potential electrolysis experiments of 4 in 0.1 M MeOH/MeCN at −2.35 V vs Fc+/0 gave a total faradaic yield close to 100%, with selectivities of 77%, 9%, and 14% for HCOOH, CO, and H2, respectively. The mechanism for CO2 reduction was studied using density functional theory, IR spectroelectrochemistry, and electrochemical methods. The results indicate that modifying the structure of the S-to-S bridge is an effective strategy to improve the catalytic performance of diiron complexes for electrocatalytic CO2 reduction.

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Diiron Complexes with Rigid and Conjugated S-to-S Bridges for Electrocatalytic Reduction of CO₂

Cheng,

Shen,

Zhang

et al. 2024

Inorg. Chem.

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Visible light-driven CO2 photoreduction by a Re(I) complex immobilized onto CuO/Nb2O5 heterojunctions

Silva,

Faustino,

Nascimento

et al. 2024

The Journal of Chemical Physics

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The immobilization of Re(I) complexes onto metal oxide surfaces presents an elegant strategy to enhance their stability and reusability toward photocatalytic CO2 reduction. In this study, the photocatalytic performance of fac-[ClRe(CO)3(dcbH2)], where dcbH2 = 4,4′-dicarboxylic acid-2,2′-bipyridine, anchored onto the surface of 1%m/m CuO/Nb2O5 was investigated. Following adsorption, the turnover number for CO production (TONCO) in DMF/TEOA increased significantly, from ten in solution to 370 under visible light irradiation, surpassing the TONCO observed for the complex onto pristine Nb2O5 or CuO surfaces. The CuO/Nb2O5 heterostructure allows for efficient electron injection by the Re(I) center, promoting efficient charge separation. At same time CuO clusters introduce a new absorption band above 550 nm that contributes for the photoreduction of the reaction intermediates, leading to a more efficient CO evolution and minimization of side reactions.

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Electrocatalytic properties of a novel ruthenium(ii) terpyridine-based complex towards CO₂ reduction

Abstract: The electrocatalytic properties of Ru complexes are of great technological interest given their potential application in reactions such water splitting and CO2 reduction. In this work, a novel terpyridine-based Ru(II)...

Cited by 2 publications

References 62 publications

Diiron Complexes with Rigid and Conjugated S-to-S Bridges for Electrocatalytic Reduction of CO₂

Diiron Complexes with Rigid and Conjugated S-to-S Bridges for Electrocatalytic Reduction of CO₂

Visible light-driven CO2 photoreduction by a Re(I) complex immobilized onto CuO/Nb2O5 heterojunctions

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Electrocatalytic properties of a novel ruthenium(ii) terpyridine-based complex towards CO2 reduction

Abstract: The electrocatalytic properties of Ru complexes are of great technological interest given their potential application in reactions such water splitting and CO2 reduction. In this work, a novel terpyridine-based Ru(II)...

Cited by 2 publications

References 62 publications

Diiron Complexes with Rigid and Conjugated S-to-S Bridges for Electrocatalytic Reduction of CO2

Diiron Complexes with Rigid and Conjugated S-to-S Bridges for Electrocatalytic Reduction of CO2

Visible light-driven CO2 photoreduction by a Re(I) complex immobilized onto CuO/Nb2O5 heterojunctions

Contact Info

Product

Resources

About

Electrocatalytic properties of a novel ruthenium(ii) terpyridine-based complex towards CO₂ reduction

Diiron Complexes with Rigid and Conjugated S-to-S Bridges for Electrocatalytic Reduction of CO₂

Diiron Complexes with Rigid and Conjugated S-to-S Bridges for Electrocatalytic Reduction of CO₂