Cubic Mo6S8-Efficient Electrocatalyst Towards Hydrogen Evolution Over Wide pH Range

Naik, Keerti M.; Sampath, S.

doi:10.1016/j.electacta.2017.09.015

Cited by 30 publications

(27 citation statements)

References 51 publications

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“…The overpotentials at 10 mA cm –2 for the traces in Figure are −0.04 (Pt), −0.23 (n-CP), −0.3 (IL-MoS 2 ), −0.67 (bulk-CP), and −0.86 (glassy carbon electrode) V versus RHE. Thus, our n-CP significantly outperforms other Chevrel phase samples from the literature where a potential of 0.32 V at 10 mA cm –2 has twice been reported. , Additionally, the overpotential of n-CP is ∼0.07 V more positive than that of IL-MoS 2 , which indicates that n-CP surface sites possess higher activity, assuming equal accessibility.…”

Section: Resultsmentioning

confidence: 51%

Chevrel Phase Nanoparticles as Electrocatalysts for Hydrogen Evolution

Strachan

Masters

Maschmeyer

2021

ACS Appl. Nano Mater.

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Chevrel phases (M x Mo6S8) are a class of molybdenum chalcogenide materials that are attractive candidates for active non-noble metal catalysts due to the relatively low coordination of their molybdenum moieties. Conventionally, the lengthy and energy-intensive synthesis of Chevrel phases (CPs) produces highly crystalline, low surface area materials. In this work, a synthetic approach leading to a Chevrel phase with an unprecedented nanostructure is presented. The resultant material is fully characterized using a variety of spectroscopic, microscopic, and electrochemical techniques. In electrochemical testing aimed at catalyzing the hydrogen evolution reaction (HER), this nanostructured catalyst shows a substantially lower overpotential than an equivalent MoS2 phase with a similar nanostructure. Furthermore, the nanostructured Chevrel phases prove to be easily modified by electrochemical intercalation, which allows performance fine-tuning, revealing a family of versatile and tuneable catalysts.

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Section: Resultsmentioning

confidence: 51%

Chevrel Phase Nanoparticles as Electrocatalysts for Hydrogen Evolution

Strachan

Masters

Maschmeyer

2021

ACS Appl. Nano Mater.

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“…CP transition metal chalcogenides showed a remarkable HER efficiency, where their activity surpassed that of 2H c-MoS 2 due to the higher density of active sites, both Mo and S, and to the improved charge transfer properties which resulted in faster HER kinetics. 114,115 The presence in the structure of transition metal atoms was exploited to fine-tune the interaction energy of the chalcogen centers with the HER intermediate and improve the reaction 117 As highlighted by Ortiz-Rodri ́guez et al, 113 the electronegativity of the chalcogen atom in the CP structure is a critical parameter to optimize the HER performance. Indeed, as the electronegativity of the chalcogen atom increases (from Te to Se and S), so does its charge density, leading to a stronger X−H bond and to an easier HER energy profile.…”

Section: Multiscale Design Strategies For Group VI Transition Metal C...mentioning

confidence: 99%

Transition Metal Chalcogenides as a Versatile and Tunable Platform for Catalytic CO₂ and N₂ Electroreduction

et al. 2021

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Group VI transition metal chalcogenides are the subject of increasing research interest for various electrochemical applications such as low-temperature water electrolysis, batteries, and supercapacitors due to their high activity, chemical stability, and the strong correlation between structure and electrochemical properties. Particularly appealing is their utilization as electrocatalysts for the synthesis of energy vectors and value-added chemicals such as C-based chemicals from the CO2 reduction reaction (CO2R) or ammonia from the nitrogen fixation reaction (NRR). This review discusses the role of structural and electronic properties of transition metal chalcogenides in enhancing selectivity and activity toward these two key reduction reactions. First, we discuss the morphological and electronic structure of these compounds, outlining design strategies to control and fine-tune them. Then, we discuss the role of the active sites and the strategies developed to enhance the activity of transition metal chalcogenide-based catalysts in the framework of CO2R and NRR against the parasitic hydrogen evolution reaction (HER); leveraging on the design rules applied for HER applications, we discuss their future perspective for the applications in CO2R and NRR. For these two reactions, we comprehensively review recent progress in unveiling reaction mechanisms at different sites and the most effective strategies for fabricating catalysts that, by exploiting the structural and electronic peculiarities of transition metal chalcogenides, can outperform many metallic compounds. Transition metal chalcogenides outperform state-of-the-art catalysts for CO2 to CO reduction in ionic liquids due to the favorable CO2 adsorption on the metal edge sites, whereas the basal sites, due to their conformation, represent an appealing design space for reduction of CO2 to complex carbon products. For the NRR instead, the resemblance of transition metal chalcogenides to the active centers of nitrogenase enzymes represents a powerful nature-mimicking approach for the design of catalysts with enhanced performance, although strategies to hinder the HER must be integrated in the catalytic architecture.

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“…Chevrel phases (CPs) are pseudomolecular solid molybdenum chalcogenides that have shown promise for a variety of applications. Although first explored in the 1970s as high-temperature superconductors, , a renewed interest in these materials was catalyzed by recent demonstrations of their potential as state-of-the-art monovalent and multivalent battery electrodes, − artificial solid-electrolyte interphases (SEI), , photovoltaics, and electrocatalysts for hydrogen evolution, − oxygen reduction, and CO 2 reduction. , The breadth of CP applications arises from their highly tunable electronic and thermodynamic properties (e.g., band gap, , band edge positions, , storage capacity, ionic transport) enabled by varying their composition (Figure a). Many thousands of multinary CP compositions are possible and are described by the general formula M y Mo 6 X 8 (0 ≤ y ≤ 4), where M is an alkali, alkaline-earth metal, transition metal (TM), post-TM, lanthanide, or combinations thereof, and X is a chalcogen (S, Se, Te) or combination of chalcogens.…”

Section: Introductionmentioning

confidence: 99%

Machine Learning Guided Synthesis of Multinary Chevrel Phase Chalcogenides

et al. 2021

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The Chevrel phase (CP) is a class of molybdenum chalcogenides that exhibit compelling properties for next-generation battery materials, electrocatalysts, and other energy applications. Despite their promise, CPs are underexplored, with only ∼100 compounds synthesized to date due to the challenge of identifying synthesizable phases. We present an interpretable machine-learned descriptor (H δ) that rapidly and accurately estimates decomposition enthalpy (ΔH d) to assess CP stability. To develop H δ, we first used density functional theory to compute ΔH d for 438 CP compositions. We then generated >560 000 descriptors with the new machine learning method SIFT, which provides an easy-to-use approach for developing accurate and interpretable chemical models. From a set of >200 000 compositions, we identified 48 501 CPs that H δ predicts are synthesizable based on the criterion that ΔH d < 65 meV/atom, which was obtained as a statistical boundary from 67 experimentally synthesized CPs. The set of candidate CPs includes 2307 CP tellurides, an underexplored CP subset with a predicted preference for channel site occupation by cation intercalants that is rare among CPs. We successfully synthesized five of five novel CP tellurides attempted from this set and confirmed their preference for channel site occupation. Our joint computational and experimental approach for developing and validating screening tools that enable the rapid identification of synthesizable materials within a sparse class is likely transferable to other materials families to accelerate their discovery.

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Cubic Mo6S8-Efficient Electrocatalyst Towards Hydrogen Evolution Over Wide pH Range

Cited by 30 publications

References 51 publications

Chevrel Phase Nanoparticles as Electrocatalysts for Hydrogen Evolution

Chevrel Phase Nanoparticles as Electrocatalysts for Hydrogen Evolution

Transition Metal Chalcogenides as a Versatile and Tunable Platform for Catalytic CO₂ and N₂ Electroreduction

Machine Learning Guided Synthesis of Multinary Chevrel Phase Chalcogenides

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Cubic Mo6S8-Efficient Electrocatalyst Towards Hydrogen Evolution Over Wide pH Range

Cited by 30 publications

References 51 publications

Chevrel Phase Nanoparticles as Electrocatalysts for Hydrogen Evolution

Chevrel Phase Nanoparticles as Electrocatalysts for Hydrogen Evolution

Transition Metal Chalcogenides as a Versatile and Tunable Platform for Catalytic CO2 and N2 Electroreduction

Machine Learning Guided Synthesis of Multinary Chevrel Phase Chalcogenides

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Transition Metal Chalcogenides as a Versatile and Tunable Platform for Catalytic CO₂ and N₂ Electroreduction