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16 pages, 4463 KB

Open AccessArticle

Electrocatalytic Hydrogen Evolution Reaction of Cobalt Triaryl Corrole Bearing Nitro Group

by Jie Zeng, Xu-You Cao, Shi-Yin Xu, Yi-Feng Qiu, Jun-Ying Chen, Li-Ping Si and Hai-Yang Liu

Catalysts 2024, 14(7), 454; https://doi.org/10.3390/catal14070454 - 15 Jul 2024

Cited by 14 | Viewed by 2939

Abstract

The use of non–precious metals for electrocatalytic hydrogen reaction (HER) is particularly important for energy conservation and environmental protection. In this work, three new cobalt corroles containing o−, m−, and p−nitrobenzyl (1, 2, 3) at the meso 10−position of the corrole macrocycle were synthesized, and their electrocatalytic hydrogen evolution reaction in organic and neutral aqueous systems was also investigated. The results show that these three cobalt corroles have significant catalytic HER activity in both systems, and the catalytic efficiency follows 1 > 3 > 2, which indicates that the position of the nitro group can affect the catalytic property of the complexes. In the organic phase, when using trifluoroacetic acid or p−toluenesulfonic acid as the proton source, the electrocatalytic HER may undergo an EECC (E: electron transfer, C: proton coupling) pathway. In a neutral aqueous system, the HER turnover frequency value of 1 is up to 137.4 h⁻¹ at 938 mV overpotential. Full article

(This article belongs to the Section Electrocatalysis)

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16 pages, 3129 KB

Open AccessArticle

Electrocatalytic Hydrogen Evolution of Transition Metal (Fe, Co and Cu)–Corrole Complexes Bearing an Imidazole Group

by Ling-Wei Wu, Yan-Fang Yao, Shi-Yin Xu, Xu-You Cao, Yan-Wei Ren, Li-Ping Si and Hai-Yang Liu

Catalysts 2024, 14(1), 5; https://doi.org/10.3390/catal14010005 - 19 Dec 2023

Cited by 21 | Viewed by 4580

Abstract

The study of the hydrogen evolution reaction (HER) by non-noble transition metals is of great significance for the production of hydrogen energy. In this work, a new 5,15-bis-(pentafluorophenyl)-10-[4-(1H-imidazole) phenyl]-corrole and its metal complexes (metal = Co, Cu, Fe) were synthesized and used for electrocatalyzed HER in DMF organic solvent and aqueous media. The prepared cobalt corrole showed the best catalytic performance in both media. Its turnover frequency (TOF) and catalytic efficiency (C.E) could reach 265 s⁻¹ and 1.04 when TsOH was used as the proton source in a DMF solvent. In aqueous media, its TOF could also reach 405 h⁻¹. The catalytic HER may go through an EECEC or ECEC (E: electron transfer, C: chemical step) pathway for these catalysts, depending on the acidity and concentration of the proton source. The present work successfully demonstrates that imidazole at a meso-phenyl group may improve the electrocatalytic HER activity of transition metal corroles. Full article

(This article belongs to the Special Issue Advanced Electrocatalytic Materials for Polymer Electrolyte Water Electrolyzers and Metal–Air Batteries)

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12 pages, 7013 KB

Open AccessArticle

Reactivity of Myoglobin Reconstituted with Cobalt Corrole toward Hydrogen Peroxide

by Koji Oohora, Hirotaka Tomoda and Takashi Hayashi

Int. J. Mol. Sci. 2022, 23(9), 4829; https://doi.org/10.3390/ijms23094829 - 27 Apr 2022

Cited by 8 | Viewed by 3665

Abstract

The protein matrix of natural metalloenzymes regulates the reactivity of metal complexes to establish unique catalysts. We describe the incorporation of a cobalt complex of corrole (CoCor), a trianionic porphyrinoid metal ligand, into an apo-form of myoglobin to provide a reconstituted protein (rMb(CoCor)). This protein was characterized by UV-vis, EPR, and mass spectroscopic measurements. The reaction of rMb(CoCor) with hydrogen peroxide promotes an irreversible oxidation of the CoCor cofactor, whereas the same reaction in the presence of a phenol derivative yields the cation radical form of CoCor. Detailed kinetic investigations indicate the formation of a transient hydroperoxo complex of rMb(CoCor) which promotes the oxidation of the phenol derivatives. This mechanism is significantly different for native heme-dependent peroxidases, which generate a metal-oxo species as an active intermediate in a reaction with hydrogen peroxide. The present findings of unique reactivity will contribute to further design of artificial metalloenzymes. Full article

(This article belongs to the Special Issue Natural, Designed and Engineered Metalloenzymes: Structure, Catalytic Mechanisms and Applications)

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16 pages, 2268 KB

Open AccessArticle

Generation of Cobalt-Containing Nanoparticles on Carbon via Pyrolysis of a Cobalt Corrole and Its Application in the Hydrogenation of Nitroarenes

by Jessica Michalke, Michael Haas, Dominik Krisch, Thomas Bögl, Stephan Bartling, Nils Rockstroh, Wolfgang Schöfberger and Christoph Topf

Catalysts 2022, 12(1), 11; https://doi.org/10.3390/catal12010011 - 23 Dec 2021

Cited by 9 | Viewed by 4937

Abstract

We report on the manufacture of a state-of-the-art heterogeneous non-noble metal catalyst, which is based on a molecularly well-defined phosphine-tagged cobalt corrole complex. This precursor compound is readily synthesized from convenient starting materials while the active material is obtained through wet-impregnation of the pertinent metalliferous macrocycle onto carbon black followed by controlled pyrolysis of the loaded carrier material under an inert gas atmosphere. Thus, the obtained composite was then applied in the heterogeneous hydrogenation of various nitroarenes to yield a vast array of valuable aniline derivatives that were conveniently isolated as their hydrochloride salts. The introduced catalytic protocol is robust and user-friendly with the entire assembly of the reaction set-up enabling the conduction of the experiments on the laboratory bench without any protection from air. Full article

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4 pages, 592 KB

Open AccessProceeding Paper

Surface Acoustic Wave Sensors for the Detection of Hazardous Compounds in Indoor Air

by Meddy Vanotti, Christophe Theron, Sacha Poisson, Valentin Quesneau, Mario Naitana, Valérie Soumann, Stéphane Brandès, Nicolas Desbois, Claude Gros, Thu-Hoa Tran-Thi and Virginie Blondeau-Patissier

Proceedings 2017, 1(4), 444; https://doi.org/10.3390/proceedings1040444 - 24 Aug 2017

Cited by 5 | Viewed by 3068

Abstract

In this work, the authors show the capabilities of Surface Acoustic Wave (SAW) devices coupled with various absorbents to probe the properties of gas sensitive materials for the manufacturing of hazardous gas sensors. The great capabilities of cobalt corroles for the trapping of carbon monoxide (CO) were exploited to produce selective sensors. These corroles were deposited on SAW delay lines surfaces and then exposed to carbon monoxide (CO) in standard conditions. Concentrations of a few hundreds of ppb were measured emphasizing the interest of such sensors for the detection of CO. Another type of sensitive layers exhibiting specific porosity adapted to the trapping of formaldehyde (CH₂O) were deposited on similar delay lines. A detection threshold of 140 ppb was shown. These encouraging results pave the way for the development of a functionalized SAW sensors network for multi-gas detection in indoor air. Full article

(This article belongs to the Proceedings of Proceedings of Eurosensors 2017, Paris, France, 3–6 September 2017)

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