Water oxidation electrocatalysis using ruthenium coordination oligomers adsorbed on multiwalled carbon nanotubes

Hoque, Asmaul; Gil‐Sepulcre, Marcos; Aguirre, Adiran de; Elemans, Johannes A. A. W.; Moonshiram, Dooshaye; Matheu, Roc; Shi, Yuanyuan; Benet‐Buchholz, Jordi; Sala, Xavier; Malfois, Marc; Solano, Eduardo; Lim, Joohyun; Manjón, Alba Garzón; Scheu, Christina; Lanza, Mario; Maseras, Feliu; Gimbert‐Suriñach, Carolina; Llobet, Antonio

doi:10.1038/s41557-020-0548-7

Cited by 78 publications

(130 citation statements)

References 59 publications

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“…[ 15 ] As this metallomacrocycle comprises three linear aromatic linker ligands in addition to the three bda units, we assumed that it should be possible to anchor this catalyst on CNTs by non‐covalent π–π and CH–π interactions toward the graphene‐like surface without further functionalization for heterogeneous catalytic water oxidation. [ 16 ] Here we report that MC3 indeed adheres to CNTs as confirmed by electrochemical techniques and atomic force microscopy (AFM). More importantly, CNT‐anchored MC3 immobilized on glassy carbon electrodes performed outstanding catalytic activity in electrochemically driven water oxidation underlining its potential for device application.…”

Section: Figurementioning

confidence: 74%

“…[8a] Thus, the observed j max value for anchored and activated MC3 is the highest one reported so far for Ru(bda) catalysts with confirmed molecular active species and comparable with the very recently observed maximum current density of 240 mA cm −2 for an immobilized Ru(tda) polymer. [16] Proven to be highly efficient, the stability and efficiency of the act-MC3@CNT@GC electrodes was then investigated by controlled potential electrolysis (CPE) experiments (Figure 3). A two-compartment setup was used, where the working and the reference electrodes were placed in one chamber and the counter electrode in the other one.…”

Section: Doi: 101002/aenm202002329mentioning

confidence: 99%

Section: Figurementioning

confidence: 99%

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Efficient Electrochemical Water Oxidation by a Trinuclear Ru(bda) Macrocycle Immobilized on Multi‐Walled Carbon Nanotube Electrodes

Schindler

Gil‐Sepulcre

Lindner³

et al. 2020

Advanced Energy Materials

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Catalytic water splitting is a viable process for the generation of renewable fuels. Here it is reported for the first time that a trinuclear supramolecular Ru(bda) (bda: 2,2′‐bipyridine‐6,6′‐dicarboxylate) catalyst, anchored on multi‐walled carbon nanotubes and subsequently immobilized on glassy carbon electrodes, shows outstanding performance in heterogeneous water oxidation. Activation of the catalyst on anodes by repetitive cyclic voltammetry (CV) scans results in a catalytic current density of 186 mA cm−2 at a potential of 1.45 V versus NHE. The activated catalyst performs water oxidation at an onset overpotential of 330 mV. The remarkably high stability of the hybrid anode is demonstrated by X‐ray absorption spectroscopy and electrochemically, revealing the absence of any degradation after 1.8 million turnovers. Foot of the wave analysis of CV data of activated electrodes with different concentrations of catalyst indicates a monomolecular water nucleophilic attack mechanism with an apparent rate constant of TOFmax (turnover frequency) of 3200 s−1.

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Section: Figurementioning

confidence: 74%

Section: Doi: 101002/aenm202002329mentioning

confidence: 99%

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Efficient Electrochemical Water Oxidation by a Trinuclear Ru(bda) Macrocycle Immobilized on Multi‐Walled Carbon Nanotube Electrodes

Schindler

Gil‐Sepulcre

Lindner³

et al. 2020

Advanced Energy Materials

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“…The calculated adsorption energy is of 11.2 kcal/mol that corresponds to an average of 5.6 kcal/mol per CH-π interaction that is in agreement with those previously reported data. 38,40,45,46 An electronic density map of the interaction between the g-C3N4 surface and the pyrene group of the Co-PYN5 catalyst is provided in the SI (Figure S5). The new hybrid material was further characterized by powder X-ray diffraction (PXRD; Figure S6), diffuse reflectance spectroscopy (DRS; Figure S7) and X-ray photoelectron spectroscopy (XPS;…”

Section: Resultsmentioning

confidence: 99%

CH-π interaction boosts photocatalytic CO2 reduction activity in a noble-metal-free system with a molecular cobalt catalyst anchored on carbon nitride

Wang

Sepulcre

Huang

et al. 2021

Preprint

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The construction of efficient noble-metal-free systems for visible-light-driven CO2 reduction still remains a key challenge. Here we report an efficient molecular hybrid system composed of a Co-PYN5 catalyst that contains a pyrene functionality that anchors on g-C3N4 dye surface via CH-π interactions. This hybrid material achieves high TONs and TOFs for visible light reduction of CO2 to CO of 533 and 95 h -1 , that are within the best reported up to now. The exceptional performance is rationalized in terms of the electronic coupling that takes place with the π-system of the pyrene group with both the g-C3N4 surface and the Co-pyridyl moiety of the catalysts.

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“…[ 63 ] Finally, one of the most impressive results in the area of polymer catalysts has been through an oligomerization technique using 4,4′‐bipyrdyl between ruthenium catalysts that catalyze water oxidation with high current densities at neutral pH on CNTs. [ 64 ]…”

Section: Heterogeneous Woc With Molecular Catalystsmentioning

confidence: 99%

Heterogeneous Water Oxidation Catalysts for Molecular Anodes and Photoanodes

et al. 2021

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Water oxidation is a critical half reaction in alternative energy and essential to producing solar fuels from light‐driven water splitting. Molecular complexes, especially those based on ruthenium, represent a promising class of catalysts for use in these systems. Studies of ruthenium complexes in homogeneous solutions represent an overwhelming majority of the literature on molecular catalysts thus far. Nonetheless, the development of devices for light‐driven water splitting necessitates the translation of catalysts to surfaces, namely, semiconductor metal‐oxide surfaces. Progress in this equally important area of heterogeneous molecular water oxidation and mechanistic studies at surfaces is reviewed herein.

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Water oxidation electrocatalysis using ruthenium coordination oligomers adsorbed on multiwalled carbon nanotubes

Cited by 78 publications

References 59 publications

Efficient Electrochemical Water Oxidation by a Trinuclear Ru(bda) Macrocycle Immobilized on Multi‐Walled Carbon Nanotube Electrodes

Efficient Electrochemical Water Oxidation by a Trinuclear Ru(bda) Macrocycle Immobilized on Multi‐Walled Carbon Nanotube Electrodes

CH-π interaction boosts photocatalytic CO2 reduction activity in a noble-metal-free system with a molecular cobalt catalyst anchored on carbon nitride

Heterogeneous Water Oxidation Catalysts for Molecular Anodes and Photoanodes

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