Molecular stabilization of chemically exfoliated bare MnPS<sub>3</sub> layers

Brotons-Alcázar, Isaac; Torres‐Cavanillas, Ramón; Morant‐Giner, Marc; Cvikl, Martin; Mañas‐Valero, Samuel; Forment‐Aliaga, Alicia; Coronado, Eugenio

doi:10.1039/d1dt02536h

Cited by 11 publications

(26 citation statements)

References 31 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…The latter modification results in significant lowering of | Δ G H * | . The obtained results ( | Δ G H * | = 0.69 eV and | Δ G H * | = 0.41 eV for V S2 @2L and V Se2 @2L, respectively (Figure a,b)), correlate with the experimental data obtained for the MnPX 3 flakes, which are in the range between 0.525 and 0.835 V, depending on X. , Thus, according to the results of our calculations, pristine MnPX 3 exhibits significant positive values of | Δ G H * | , which can be reduced by introducing a defect. To further lower the | Δ G H * | value, doping with heteroatoms – metallic and non-metallic – can be used.…”

Section: Resultssupporting

confidence: 88%

“…Following many experimental and theoretical works on 2D materials and the respective interest to renewable energy sources, in the past decade, significant attention is given to van der Waals layered materials known as transition metal trichalcogenides (MPX 3 with M: transition metal and X: S or Se). − From the crystallographic point of view, these materials are similar to transition metal dichalcogenides, MX 2 , where one-third of the metal cations with connected X-anions is substituted by an ethane-like [P 2 X 6 ] 4– unit (Figure a,b). The diversity in transition metals and two different chalcogens can lead to a wide variation in the electronic and magnetic properties of these materials, − which can be further tailored by applying stress, an external voltage gate, , or by alloying. , Due to the layered structure of MPX 3 , they can be easily prepared as two-dimensional nanostructures , with a large surface area and high number of active sites. ,− Consequently, the MPX 3 materials have been the subject of several application-related investigations, ,,,, and FePSe 3 and MnPSe 3 yielded the highest efficiency for HER and very good stability in a wide pH range. At that, the existing theoretical and experimental works, focused on the electrocatalytic properties of MPX 3 , very rarely contain an insight in the electronic structure, which is crucial for understanding and controllable modification of the catalytic activity of these materials.…”

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Probing Active Sites on Pristine and Defective MnPX₃ (X: S and Se) Monolayers for Electrocatalytic Water Splitting

Dai,

Wang,

Voloshina

et al. 2023

ACS Omega

View full text Add to dashboard Cite

The state-of-the-art density functional theory approach was used to study the structural and electronic properties of pristine and defective MnPX 3 monolayers as well as their activity toward water and hydrogen evolution reaction (HER) catalytic performance. The adsorption behavior of H 2 O on a pristine MnPX 3 structure is of physisorption nature, whereas the adsorption energy is significantly increased for the defective structures. At the same time, the water dissociation process is more energetically favorable, and the reactivity of MnPX 3 is determined by the vacancy configuration. Following Nørskov's approach, the HER catalytic performance is evaluated by calculating the hydrogen adsorption free energy on the respective MnPX 3 surface. Our calculation results demonstrate that defective 2D MnPX 3 with low coordinated P shows significantly higher HER performance compared to the pristine counterpart.

show abstract

Section: Resultssupporting

confidence: 88%

Section: Introductionmentioning

confidence: 99%

Probing Active Sites on Pristine and Defective MnPX₃ (X: S and Se) Monolayers for Electrocatalytic Water Splitting

Dai,

Wang,

Voloshina

et al. 2023

ACS Omega

View full text Add to dashboard Cite

show abstract

“…These results quantitatively agree with reports in literature for other wet methods. 28 Note that the significant advantage of the present method is that no electrolytes, intercalating agents, additional washing steps, nor temperature annealing 27 − 29 , 40 , 41 of the collected supernatant have been employed, leaving the material unaltered and the surface clean for further chemical functionalization.…”

Section: Resultsmentioning

confidence: 99%

Direct Magnetic Evidence, Functionalization, and Low-Temperature Magneto-Electron Transport in Liquid-Phase Exfoliated FePS₃

et al. 2023

View full text Add to dashboard Cite

Magnetism and the existence of magnetic order in a material is determined by its dimensionality. In this regard, the recent emergence of magnetic layered van der Waals (vdW) materials provides a wide playground to explore the exotic magnetism arising in the two-dimensional (2D) limit. The magnetism of 2D flakes, especially antiferromagnetic ones, however, cannot be easily probed by conventional magnetometry techniques, being often replaced by indirect methods like Raman spectroscopy. Here, we make use of an alternative approach to provide direct magnetic evidence of few-layer vdW materials, including antiferromagnets. We take advantage of a surfactant-free, liquid-phase exfoliation (LPE) method to obtain thousands of few-layer FePS3 flakes that can be quenched in a solvent and measured in a conventional SQUID magnetometer. We show a direct magnetic evidence of the antiferromagnetic transition in FePS3 few-layer flakes, concomitant with a clear reduction of the Néel temperature with the flake thickness, in contrast with previous Raman reports. The quality of the LPE FePS3 flakes allows the study of electron transport down to cryogenic temperatures. The significant through-flake conductance is sensitive to the antiferromagnetic order transition. Besides, an additional rich spectra of electron transport excitations, including secondary magnetic transitions and potentially magnon-phonon hybrid states, appear at low temperatures. Finally, we show that the LPE is additionally a good starting point for the mass covalent functionalization of 2D magnetic materials with functional molecules. This technique is extensible to any vdW magnetic family.

show abstract

“…The complementary question, i.e., how the 2D material affects the properties of the SCO component, has not been investigated so far. [ 25,26 ]…”

Section: Introductionmentioning

confidence: 99%

Hybrid Heterostructures of a Spin Crossover Coordination Polymer on MoS₂: Elucidating the Role of the 2D Substrate

Núñez‐López,

Torres‐Cavanillas,

Morant‐Giner

et al. 2023

Small

Self Cite

View full text Add to dashboard Cite

Controlling the deposition of spin‐crossover (SCO) materials constitutes a crucial step for the integration of these bistable molecular systems in electronic devices. Moreover, the influence of functional surfaces, such as 2D materials, can be determinant on the properties of the deposited SCO film. In this work, ultrathin films of the SCO Hofmann‐type coordination polymer [Fe(py)2{Pt(CN)4}] (py = pyridine) onto monolayers of 1T and 2H MoS2 polytypes are grown. The resulting hybrid heterostructures are characterized by GIXRD, XAS, XPS, and EXAFS to get information on the structure and the specific interactions generated at the interface, as well as on the spin transition. The use of a layer‐by‐layer results in SCO/2D heterostructures, with crystalline and well‐oriented [Fe(py)2{Pt(CN)4}]. Unlike with conventional Au or SiO2 substrates, no intermediate self‐assembled monolayer is required, thanks to the surface S atoms. Furthermore, it is observed that the higher presence of Fe3+ in the 2H heterostructures hinders an effective spin transition for [Fe(py)2{Pt(CN)4}] films thinner than 8 nm. Remarkably, when using 1T MoS2, this transition is preserved in films as thin as 4 nm, due to the reducing character of this metallic substrate. These results highlight the active role that 2D materials play as substrates in hybrid molecular/2D heterostructures.

show abstract

Molecular stabilization of chemically exfoliated bare MnPS₃ layers

Abstract: Transition metal chalcogenophosphates of general formula MPX3 have attracted recent interest in the field of 2D materials due to the possibility of tuning their properties when reaching the 2D limit....

Cited by 11 publications

References 31 publications

Probing Active Sites on Pristine and Defective MnPX₃ (X: S and Se) Monolayers for Electrocatalytic Water Splitting

Probing Active Sites on Pristine and Defective MnPX₃ (X: S and Se) Monolayers for Electrocatalytic Water Splitting

Direct Magnetic Evidence, Functionalization, and Low-Temperature Magneto-Electron Transport in Liquid-Phase Exfoliated FePS₃

Hybrid Heterostructures of a Spin Crossover Coordination Polymer on MoS₂: Elucidating the Role of the 2D Substrate

Contact Info

Product

Resources

About

Molecular stabilization of chemically exfoliated bare MnPS3 layers

Abstract: Transition metal chalcogenophosphates of general formula MPX3 have attracted recent interest in the field of 2D materials due to the possibility of tuning their properties when reaching the 2D limit....

Cited by 11 publications

References 31 publications

Probing Active Sites on Pristine and Defective MnPX3 (X: S and Se) Monolayers for Electrocatalytic Water Splitting

Probing Active Sites on Pristine and Defective MnPX3 (X: S and Se) Monolayers for Electrocatalytic Water Splitting

Direct Magnetic Evidence, Functionalization, and Low-Temperature Magneto-Electron Transport in Liquid-Phase Exfoliated FePS3

Hybrid Heterostructures of a Spin Crossover Coordination Polymer on MoS2: Elucidating the Role of the 2D Substrate

Contact Info

Product

Resources

About

Molecular stabilization of chemically exfoliated bare MnPS₃ layers

Probing Active Sites on Pristine and Defective MnPX₃ (X: S and Se) Monolayers for Electrocatalytic Water Splitting

Probing Active Sites on Pristine and Defective MnPX₃ (X: S and Se) Monolayers for Electrocatalytic Water Splitting

Direct Magnetic Evidence, Functionalization, and Low-Temperature Magneto-Electron Transport in Liquid-Phase Exfoliated FePS₃

Hybrid Heterostructures of a Spin Crossover Coordination Polymer on MoS₂: Elucidating the Role of the 2D Substrate