Mechanistic insights of molecular metal polyselenides for catalytic hydrogen generation

Elliott, Alexander; McAllister, James; Masaityte, Liudvika; Segado, Mireia; Long, De‐Liang; Ganin, Alexey Y.; Song, Yu‐Fei; Bó, Carles; Miras, Haralampos N.

doi:10.1039/d2cc01226j

Cited by 3 publications

(4 citation statements)

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“…The difference in electronegativity of sulphur and selenium is smaller, however it is still large enough to manifest as a 0.1 V difference in the standard reduction potential of the E/E 2− couple [24] . It is further observed that structures containing the [Mo V 2 (μ‐O) 2 O 2 ] 2+ motif are invariably supported by negatively charged ligands [1, 25–29] coordinated to the axial position, whilst the [Mo V 2 (μ‐S) 2 O 2 ] 2+ and [Mo V 2 (μ‐Se) 2 O 2 ] 2+ are found supported by water [30, 31] on their axial positions, or with uncoordinated axial positions [32, 33, 34] …”

Section: Resultsmentioning

confidence: 98%

“… [24] It is further observed that structures containing the [Mo V 2 (μ‐O) 2 O 2 ] 2+ motif are invariably supported by negatively charged ligands[ 1 , 25 , 26 , 27 , 28 , 29 ] coordinated to the axial position, whilst the [Mo V 2 (μ‐S) 2 O 2 ] 2+ and [Mo V 2 (μ‐Se) 2 O 2 ] 2+ are found supported by water[ 30 , 31 ] on their axial positions, or with uncoordinated axial positions. [ 32 , 33 , 34 ]…”

Section: Resultsmentioning

confidence: 99%

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Pore “Softening” and Emergence of Breathability Effects of New Keplerate Nano‐Containers

et al. 2023

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The self‐assembly of porous molecular nanocapsules offer unique opportunities to investigate a range of interesting phenomena and applications. However, to design nanocapsules with pre‐defined properties, thorough understanding of their structure‐property relation is required. Here, we report the self‐assembly of two elusive members of the Keplerate family, [Mo132Se60O312(H2O)72(AcO)30]42− {Mo132Se60} 1 and [W72Mo60Se60O312(H2O)72(AcO)30]42− {W72Mo60Se60} 2, that have been synthesised using pentagonal and dimeric ([Mo2O2Se2]2+) building blocks and their structures have been confirmed via single crystal X‐ray diffractions. Our comparative study involving the uptake of organic ions and the related ligand exchange of various ligand sizes by the {Mo132Se60} and previously reported Keplerates {Mo132O60}, {Mo132S60} based on the ligand exchange rates, revealed the emergence of increased “breathability” that dominates over the pore size as we transition from the {Mo132S60} to the “softer” {Mo132Se60} molecular nano‐container.

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Section: Resultsmentioning

confidence: 98%

Section: Resultsmentioning

confidence: 99%

Pore “Softening” and Emergence of Breathability Effects of New Keplerate Nano‐Containers

et al. 2023

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“…This includes research on other types of thiometalates, such as thiotungstates, [ 33 ] mixed‐ligand clusters, e.g., featuring oxo‐ or organic ligands in addition to thio groups, [ 17 ] as well as selenide‐containing derivatives. [ 110 ] While these areas are highly promising, they have thus far not received the attention to allow us to draw any final conclusions on the component suitability for HER studies.…”

Section: Discussionmentioning

confidence: 99%

Thiomolybdate Clusters: From Homogeneous Catalysis to Heterogenization and Active Sites

Batool,

Langer,

Myakala

et al. 2023

Advanced Materials

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Thiomolybdates are molecular molybdenum‐sulfide clusters formed from Mo centers and sulfur‐based ligands. For decades, they have attracted the interest of synthetic chemists due to their unique structures and their relevance in biological systems, e.g., as reactive sites in enzymes. More recently, thiomolybdates have been explored from the catalytic point of view and applied as homogeneous and molecular mimics of heterogeneous molybdenum sulfide catalysts. This review summarizes prominent examples of thiomolybdate‐based electro‐ and photocatalysis and provides a comprehensive analysis of their reactivities under homogeneous and heterogenized conditions. Active sites of thiomolybdates relevant for the hydrogen evolution reaction (HER) are examined, aiming to shed light on the link between cluster structure and performance. The shift from solution‐phase to surface‐supported thiomolybdates is discussed with a focus on applications in electrocatalysis and photocatalysis. The outlook highlights current trends and emerging areas of thiomolybdate research, ending with a summary of challenges and key takeaway messages based on the state‐of‐the‐art research.This article is protected by copyright. All rights reserved

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“…[24] It is further observed that structures containing the [Mo V 2 (μ-O) 2 O 2 ] 2 + motif are invariably supported by negatively charged ligands [1,[25][26][27][28][29] coordinated to the axial position, whilst the [Mo V 2 (μ-S) 2 O 2 ] 2 + and [Mo V 2 (μ-Se) 2 O 2 ] 2 + are found supported by water [30,31] on their axial positions, or with uncoordinated axial positions. [32,33,34]…”

Section: Forschungsartikelmentioning

confidence: 99%

Pore “Softening” and Emergence of Breathability Effects of New Keplerate Nano‐Containers

et al. 2023

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Mechanistic insights of molecular metal polyselenides for catalytic hydrogen generation

Abstract: Molecular metal chalcogenides have attracted great attention as electrocatalysts for the hydrogen evolution reaction (HER). However, efficient utilisation of the active sites and catalytic performance modulation has been challenging. Here...

Cited by 3 publications

References 25 publications

Pore “Softening” and Emergence of Breathability Effects of New Keplerate Nano‐Containers

Pore “Softening” and Emergence of Breathability Effects of New Keplerate Nano‐Containers

Thiomolybdate Clusters: From Homogeneous Catalysis to Heterogenization and Active Sites

Pore “Softening” and Emergence of Breathability Effects of New Keplerate Nano‐Containers

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