Metall‐Phosphor‐Trichalkogenide (MPCh<sub>3</sub>): von der Synthese zu aktuellen Energieanwendungen

Gusmão, Rui; Sofer, Zdeněk; Pumera, Martin

doi:10.1002/ange.201810309

Angewandte Chemie

2019

DOI: 10.1002/ange.201810309

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Metall‐Phosphor‐Trichalkogenide (MPCh₃): von der Synthese zu aktuellen Energieanwendungen

Rui Gusmão

Zdeněk Sofer

Martin Pumera

Abstract: Aufgrund ihrer speziellen physikalischen und chemischen Eigenschaften stehen zweidimensionale (2D‐)Schichtmaterialien im Fokus der aktuellen materialwissenschaftlichen Forschung. Dies schließt Schichten ein, die aus einem einzelnen Element (Graphen, Phosphoren), zwei Elementen (Metall‐Dichalkogenide) oder mehreren Elementen bestehen. Die erstmals im späten 19. Jahrhundert synthetisierten Metall‐Phosphor‐Trichalkogenide (MPCh3 mit Ch=S, Se) bilden eine besondere Klasse von 2D‐Schichtmaterialien. MPCh3‐Verbindun… Show more

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Cited by 5 publications

References 82 publications

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Expediting Oxygen Evolution by Optimizing Cation and Anion Complexity in Electrocatalysts Based on Metal Phosphorous Trichalcogenides

Liu

Dong

et al. 2023

Angewandte Chemie

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Purposely changing the rate-determining step (RDS) of oxygen evolution reaction (OER) remains a major challenge for enhancing the energy efficiency of electrochemical splitting of water. Here we show that the OER RDS can be regulated by simply varying the cation and anion complexity in a family of the metal phosphorous trichalcogenide electrocatalysts (MPT 3 , where M = Fe, Ni; T = S, Se), achieving an exceptionally high OER activity in (Ni,Fe)P(S,Se) 3 , as demonstrated by its ultra-low Tafel slope (34 mV dec À 1 ) and a very low overpotential compared to many relevant OER catalysts. This is strongly supported by density functional theory calculations, which showed that this catalyst has a nearly optimal OER activity descriptor value of ΔG-(O*)À ΔG(OH*) = 1.5 eV. We also found that the activity descriptor is proportional to a newly proposed cation/anion complexity index that consists of pairwise contributions from cation-anion bonds in a catalyst compound, revealing the pivotal role of the cation-anion interactions in determining the catalyst performance and providing a simple way for predicting catalytic activities.

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Expediting Oxygen Evolution by Optimizing Cation and Anion Complexity in Electrocatalysts Based on Metal Phosphorous Trichalcogenides

Liu

Dong

et al. 2023

Angewandte Chemie

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Exfoliated 2D Layered and Nonlayered Metal Phosphorous Trichalcogenides Nanosheets as Promising Electrocatalysts for CO₂ Reduction

Wang

Jiao

et al. 2023

Angewandte Chemie

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Two‐dimensional (2D) materials catalysts provide an atomic‐scale view on a fascinating arena for understanding the mechanism of electrocatalytic carbon dioxide reduction (CO2 ECR). Here, we successfully exfoliated both layered and nonlayered ultra‐thin metal phosphorous trichalcogenides (MPCh3) nanosheets via wet grinding exfoliation (WGE), and systematically investigated the mechanism of MPCh3 as catalysts for CO2 ECR. Unlike the layered CoPS3 and NiPS3 nanosheets, the active Sn atoms tend to be exposed on the surfaces of nonlayered SnPS3 nanosheets. Correspondingly, the nonlayered SnPS3 nanosheets exhibit clearly improved catalytic activity, showing formic acid selectivity up to 31.6 % with −7.51 mA cm−2 at −0.65 V vs. RHE. The enhanced catalytic performance can be attributed to the formation of HCOO* via the first proton‐electron pair addition on the SnPS3 surface. These results provide a new avenue to understand the novel CO2 ECR mechanism of Sn‐based and MPCh3‐based catalysts.

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Expediting Oxygen Evolution by Optimizing Cation and Anion Complexity in Electrocatalysts Based on Metal Phosphorous Trichalcogenides

Liu

Dong

et al. 2023

Angew Chem Int Ed

View full text Add to dashboard Cite

Purposely changing the rate‐determining step (RDS) of oxygen evolution reaction (OER) remains a major challenge for enhancing the energy efficiency of electrochemical splitting of water. Here we show that the OER RDS can be regulated by simply varying the cation and anion complexity in a family of the metal phosphorous trichalcogenide electrocatalysts (MPT3, where M=Fe, Ni; T=S, Se), achieving an exceptionally high OER activity in (Ni,Fe)P(S,Se)3, as demonstrated by its ultra‐low Tafel slope (34 mV dec−1) and a very low overpotential compared to many relevant OER catalysts. This is strongly supported by density functional theory calculations, which showed that this catalyst has a nearly optimal OER activity descriptor value of ΔG(O*)−ΔG(OH*)=1.5 eV. We also found that the activity descriptor is proportional to a newly proposed cation/anion complexity index that consists of pairwise contributions from cation‐anion bonds in a catalyst compound, revealing the pivotal role of the cation‐anion interactions in determining the catalyst performance and providing a simple way for predicting catalytic activities.

show abstract

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Metall‐Phosphor‐Trichalkogenide (MPCh₃): von der Synthese zu aktuellen Energieanwendungen

Cited by 5 publications

References 82 publications

Expediting Oxygen Evolution by Optimizing Cation and Anion Complexity in Electrocatalysts Based on Metal Phosphorous Trichalcogenides

Expediting Oxygen Evolution by Optimizing Cation and Anion Complexity in Electrocatalysts Based on Metal Phosphorous Trichalcogenides

Exfoliated 2D Layered and Nonlayered Metal Phosphorous Trichalcogenides Nanosheets as Promising Electrocatalysts for CO₂ Reduction

Expediting Oxygen Evolution by Optimizing Cation and Anion Complexity in Electrocatalysts Based on Metal Phosphorous Trichalcogenides

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Metall‐Phosphor‐Trichalkogenide (MPCh3): von der Synthese zu aktuellen Energieanwendungen

Cited by 5 publications

References 82 publications

Expediting Oxygen Evolution by Optimizing Cation and Anion Complexity in Electrocatalysts Based on Metal Phosphorous Trichalcogenides

Expediting Oxygen Evolution by Optimizing Cation and Anion Complexity in Electrocatalysts Based on Metal Phosphorous Trichalcogenides

Exfoliated 2D Layered and Nonlayered Metal Phosphorous Trichalcogenides Nanosheets as Promising Electrocatalysts for CO2 Reduction

Expediting Oxygen Evolution by Optimizing Cation and Anion Complexity in Electrocatalysts Based on Metal Phosphorous Trichalcogenides

Contact Info

Product

Resources

About

Metall‐Phosphor‐Trichalkogenide (MPCh₃): von der Synthese zu aktuellen Energieanwendungen

Exfoliated 2D Layered and Nonlayered Metal Phosphorous Trichalcogenides Nanosheets as Promising Electrocatalysts for CO₂ Reduction