Geoinspired syntheses of materials and nanomaterials

Portehault, David; Gómez‐Recio, Isabel; Baron, M. A.; Musumeci, Valentina; Aymonier, Cyril; Rouchon, Virgile; Godec, Yann Le

doi:10.1039/d0cs01283a

Cited by 7 publications

(3 citation statements)

References 283 publications

(416 reference statements)

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“…[41][42][43] What's more, most conventional syntheses with molten salts require washing away them at the end, which could have an impact on the surface properties of the products and adds to complication of the experiment. [44][45][46] In this case, NaCl evaporates away gradually at high temperatures after coming into play. The whole experimental process is simplified, avoiding additional impact on the products.…”

Section: Mechanism and Advantagesmentioning

confidence: 99%

New Strategy: Molten Salt‐Assisted Synthesis to Enhance Lanthanide Upconversion Luminescence

Lei

Liang

et al. 2023

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Lanthanide‐doped upconversion luminescent materials (LUCMs) have attracted much attention in diverse practical applications because of their superior features. However, the relatively weak luminescence intensity and low efficiency of LUCMs are the bottleneck problems that seriously limit their development. Unfortunately, most of the current major strategies of luminescence enhancement have some inherent shortcomings in their implementation. Here, a new and simple strategy of molten salt‐assisted synthesis is proposed to enhance lanthanide upconversion luminescence for the first time. As a proof‐of‐concept, a series of rare earth oxides with obvious luminescence enhancement are prepared by a one‐step method, utilizing molten NaCl as the high‐temperature reaction media and rare earth chlorides as the precursors. The enhancement factors at different reaction temperatures are systematically investigated by taking Yb3+/Er3+ co‐doped Y2O3 as an example, which can be enhanced up to more than six times. In addition, the molten salts are extended to all alkali chlorides, indicating that it is a universal strategy. Finally, the potential application of obtained UCL materials is demonstrated in near‐infrared excited upconversion white light‐emitting diodes (WLEDs) and other monochromatic LEDs.

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Section: Mechanism and Advantagesmentioning

confidence: 99%

New Strategy: Molten Salt‐Assisted Synthesis to Enhance Lanthanide Upconversion Luminescence

Lei

Liang

et al. 2023

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“…Our strategy consists of developing a redox chemical route within molten salts as inorganic solvents. Molten salts enable liquid-phase synthesis at temperatures higher than those accessible with usual solvents, , but lower than those traditionally employed for solids reluctant to crystallization. − Within this route, we trigger a range of new transformations with only minor atomic rearrangement of covalent frameworks, hence enabling further decrease of the synthesis temperature.…”

Section: Introductionmentioning

confidence: 99%

Covalent Transition Metal Borosilicides: Reaction Pathways in Molten Salts for Water Oxidation Electrocatalysis

Janisch,

Igoa Saldaña,

De Rolland Dalon

et al. 2024

J. Am. Chem. Soc.

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The properties of transition metal borides and silicides are intimately linked to the covalent character of the chemical bonds within their crystal structures. Bringing boron and silicon together within metal borosilicides can then engender different competing covalent networks and complex charge distributions. This situation results in unique structures and atomic environments, which can impact charge transport and catalytic properties. Metal borosilicides, however, hold the status of unusual exotic species, difficult to synthesize and with poor knowledge of their properties. Our strategy consists of developing a redox pathway to synthesize transition metal borosilicides in inorganic molten salts as high-temperature solvents. By studying the formation of Ni 6 Si 2 B, Co 4.75 Si 2 B, Fe 5 SiB 2 , and Mn 5 SiB 2 with in situ X-ray diffraction, we highlight how new reaction routes, maintaining covalent structural building blocks, draw a general scheme of their formation. This pathway is driven by the covalence of the chemical bonds within the boron coordination framework. Next, we demonstrate high efficiency for water oxidation electrocatalysis, especially for Ni 6 Si 2 B. We ascribe the strongly increased resistance to corrosion, high stability, and electrocatalytic activity of the Ni 6 Si 2 B-derived material to three factors: (1) the two entangled boron and silicon covalent networks; (2) the ability to codope with boron and silicon an in situ generated catalytic layer; and (3) a rare electron enrichment of the transition metal by back-donation from boron atoms, previously unknown within this compound family. With this work, we then unveil a new chemical dimension for Earth-abundant water oxidation electrocatalysts by bringing to light a new family of materials.

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“…First, we use molten salts media at lower temperature (420 °C) than usual flux syntheses of oxyhalides, [13,14] to avoid thermal decomposition of the product during synthesis, while enabling the recovery of metastable solids. [20] As liquid media, molten salts also increase the nucleation and crystallization rates compared to solid-state reactions, [21] thus giving access to nano-objects, [21] which are scarce among oxyhalides and exacerbate the impact of the surface on the properties, especially for catalysis. Second, we use [SiO 4 ] tetrahedral connectors already observed in the few metalsilicon oxyhalides reported (27 entries in the Inorganic Crystal Structure Database excluding Rare Earths), [17] especially in Cd 4 Si 2 O 7 F 2 , [22] which has been the only oxyhalide of silicon and a post-transition metal before the present work.…”

Section: Introductionmentioning

confidence: 99%

Molten Salts‐Driven Discovery of a Polar Mixed‐Anion 3D Framework at the Nanoscale: Zn₄Si₂O₇Cl₂, Charge Transport and Photoelectrocatalytic Water Splitting

et al. 2023

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Mixed-anion compounds widen the chemical space of attainable materials compared to single anionic compounds, but the exploration of their structural diversity is limited by common synthetic paths. Especially, oxychlorides rely mainly on layered structures, which suffer from low stability during photo(electro)catalytic processes. Herein we report a strategy to design a new polar 3D tetrahedral framework with composition Zn 4 Si 2 O 7 Cl 2 . We use a molten salt medium to enable low temperature crystallization of nanowires of this new compound, by relying on tetrahedral building units present in the melt to build the connectivity of the oxychloride. These units are combined with silicon-based connectors from a non-oxidic Zintl phase to enable precise tuning of the oxygen content. This structure brings high chemical and thermal stability, as well as strongly anisotropic hole mobility along the polar axis. These features, associated with the ability to adjust the transport properties by doping, enable to tune water splitting properties for photoelectrocatalytic H 2 evolution and water oxidation. This work then paves the way to a new family of mixed-anion solids

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Geoinspired syntheses of materials and nanomaterials

Abstract: State-of-the-art synthesis pathways towards novel inorganic materials and nanomaterials are presented in the light of their relationship with geosciences, showing how geological phenomena can inspire innovative synthesis methods and materials.

Cited by 7 publications

References 283 publications

New Strategy: Molten Salt‐Assisted Synthesis to Enhance Lanthanide Upconversion Luminescence

New Strategy: Molten Salt‐Assisted Synthesis to Enhance Lanthanide Upconversion Luminescence

Covalent Transition Metal Borosilicides: Reaction Pathways in Molten Salts for Water Oxidation Electrocatalysis

Molten Salts‐Driven Discovery of a Polar Mixed‐Anion 3D Framework at the Nanoscale: Zn₄Si₂O₇Cl₂, Charge Transport and Photoelectrocatalytic Water Splitting

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Geoinspired syntheses of materials and nanomaterials

Abstract: State-of-the-art synthesis pathways towards novel inorganic materials and nanomaterials are presented in the light of their relationship with geosciences, showing how geological phenomena can inspire innovative synthesis methods and materials.

Cited by 7 publications

References 283 publications

New Strategy: Molten Salt‐Assisted Synthesis to Enhance Lanthanide Upconversion Luminescence

New Strategy: Molten Salt‐Assisted Synthesis to Enhance Lanthanide Upconversion Luminescence

Covalent Transition Metal Borosilicides: Reaction Pathways in Molten Salts for Water Oxidation Electrocatalysis

Molten Salts‐Driven Discovery of a Polar Mixed‐Anion 3D Framework at the Nanoscale: Zn4Si2O7Cl2, Charge Transport and Photoelectrocatalytic Water Splitting

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Molten Salts‐Driven Discovery of a Polar Mixed‐Anion 3D Framework at the Nanoscale: Zn₄Si₂O₇Cl₂, Charge Transport and Photoelectrocatalytic Water Splitting