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result(s) for
"Terlier, Tanguy"
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An electrochemically stable homogeneous glassy electrolyte formed at room temperature for all-solid-state sodium batteries
All-solid-state sodium batteries (ASSSBs) are promising candidates for grid-scale energy storage. However, there are no commercialized ASSSBs yet, in part due to the lack of a low-cost, simple-to-fabricate solid electrolyte (SE) with electrochemical stability towards Na metal. In this work, we report a family of oxysulfide glass SEs (Na
3
PS
4−
x
O
x
, where 0 <
x
≤ 0.60) that not only exhibit the highest critical current density among all Na-ion conducting sulfide-based SEs, but also enable high-performance ambient-temperature sodium-sulfur batteries. By forming bridging oxygen units, the Na
3
PS
4−
x
O
x
SEs undergo pressure-induced sintering at room temperature, resulting in a fully homogeneous glass structure with robust mechanical properties. Furthermore, the self-passivating solid electrolyte interphase at the Na|SE interface is critical for interface stabilization and reversible Na plating and stripping. The new structural and compositional design strategies presented here provide a new paradigm in the development of safe, low-cost, energy-dense, and long-lifetime ASSSBs.
Single sodium-ion solid electrolyte that meets the requirements of practical applications is difficult to design. Here, the authors show how kinetic stability via the creation of a self-passivating solid electrolyte interphase allows a homogenous glass solid electrolyte to exhibit remarkable electrochemical stability with sodium metal.
Journal Article
Suppressing phase disproportionation in quasi-2D perovskite light-emitting diodes
2023
Electroluminescence efficiencies and stabilities of quasi-two-dimensional halide perovskites are restricted by the formation of multiple-quantum-well structures with broad and uncontrollable phase distributions. Here, we report a ligand design strategy to substantially suppress diffusion-limited phase disproportionation, thereby enabling better phase control. We demonstrate that extending the π-conjugation length and increasing the cross-sectional area of the ligand enables perovskite thin films with dramatically suppressed ion transport, narrowed phase distributions, reduced defect densities, and enhanced radiative recombination efficiencies. Consequently, we achieved efficient and stable deep-red light-emitting diodes with a peak external quantum efficiency of 26.3% (average 22.9% among 70 devices and cross-checked) and a half-life of ~220 and 2.8 h under a constant current density of 0.1 and 12 mA/cm
2
, respectively. Our devices also exhibit wide wavelength tunability and improved spectral and phase stability compared with existing perovskite light-emitting diodes. These discoveries provide critical insights into the molecular design and crystallization kinetics of low-dimensional perovskite semiconductors for light-emitting devices.
Quasi-2D halide perovskites are attracting increasing attention for light-emitting devices. Here, the authors demonstrated efficient and stable quasi-2D perovskite LEDs enabled by suppressed phase disproportionation with newly designed organic ligands.
Journal Article
Bio-inspired multifunctional disruptors of calcium oxalate crystallization
2025
Calcium mineralization in biological and geological systems is often regulated by (macro)molecules enriched with anionic functional moieties. Relatively few studies have examined the effects of phosphate-based modifiers that are integral in calcification underlying human bone formation and pathological diseases. Here we mimic posttranslational phosphorylated moieties of a biologically-active inhibitor protein and demonstrate that polyphosphates and phosphonates suppress calcium oxalate nucleation, tailor solvate crystal structure, and irreversibly inhibit crystal growth in ways that significantly deviate from commonly investigated carboxylate-rich modulators of biomineralization. The most potent modifiers exhibit an uncommon dual mode of action, wherein nucleation is suppressed by altering prenucleation clusters and crystal surface growth is impeded irreversibly by inducing lattice strain. Once crystal surfaces are exposed to modifiers, recrystallization is severely restricted. This exemplifies the uniqueness and efficiency of phosphates wherein their multiple modes of action are promising characteristics for designing de novo biologically-inspired molecules as mineralization regulators.
Control of crystallisation is important in biogenic and pathological biomineralisation. Here, the authors report on phosphorylated molecules that mimic proteins which can suppress calcium oxalate nucleation and irreversibly inhibit crystal growth in ways that significantly deviate from commonly investigated carboxylate-rich modulators of biomineralization.
Journal Article
The Effect of a Low Degree of Fluorine Substitution on Cotton Fiber Properties
by
Kirkensgaard, Jacob Judas Kain
,
Field, Robert A.
,
Natalio, Filipe
in
Cellulose
,
Cellulose fibers
,
Chemical reactions
2024
Cellulose modification often employs chemical processes to tailor its properties and functionalities to fit the demands of a wide range of applications, maximizing its potential as a versatile and sustainable material. From both synthetic and environmental standpoints, one of the ultimate goals is to achieve significant modifications to enhance the end properties of the cellulose while minimizing the number of modified building blocks. The current study demonstrates that a synthetic glucose derivative, 6‐deoxy‐6‐fluoro‐glucose (6F‐Glc), fed into the fertilized cotton ovules, resulted in the accumulation of fluorine inside the cotton fibers with no apparent alteration to their morphology or development. These fibers exhibited a degree of substitution of 0.006, which is 170 times lower than that reported for chemical methods for cellulose modification. However, the physical characterization of the modified fibers showed a surprisingly large impact of this low‐level modification on the cellulose structure (e.g., hydrogen bonding network rearrangement) and a modest increase in the mechanical properties of the fibers. The obtained results exemplify the use of biological systems to introduce low quantities of new functionalities while maximizing the impact on fiber properties. Feeding cotton ovule cultures with a glucose derivative (6F‐Glc) leads to fibers with an exceptionally low degree of substitution. Despite this minimal modification, the fibers exhibit a modified structure and mechanical properties, highlighting the potential of harnessing biological systems for creating functionally modified cellulose fibers.
Journal Article
Comparative evaluation of intermediate solutions in prevention of brown precipitate formed from sodium hypochlorite and chlorhexidine gluconate
by
Jeong, Ji Wook
,
Sarmast, Nima D.
,
Bueso, Vashti
in
brown precipitation
,
Chemical Precipitation
,
chlorohexidine gluconate
2022
Objectives To evaluate intermediate treatments between sodium hypochlorite and chlorhexidine gluconate irrigations for the prevention of a toxic brown precipitate in root canal therapy. Materials and Methods Thirty‐nine premolars were irrigated with 6% sodium hypochlorite and divided into either: No intermediate treatment; Dry paper points; three different irrigations with 17% ethylenediaminetetraacetic acid, deionized water, or 5% sodium thiosulfate. 2% chlorhexidine gluconate was the final irrigant in all groups. Sectioned teeth were analyzed for brown precipitate intensity and area using stereomicroscopy and components related to para‐chloroaniline using Time‐of‐Flight Secondary Ion Mass Spectrometry (ToF‐SIMS). Results Stereomicroscopy showed that 5% STS significantly reduced brown precipitate intensity and area as compared with no intermediate irrigation (p < .05, Chi‐square, generalized linear model, and Tukey's multiple comparison tests). Utilizing ToF‐SIMS, 5% sodium thiosulfate was most effective in reducing the components representing para‐chloroaniline and chlorhexidine gluconate. Conclusion The 5% sodium thiosulfate was most effective among other intermediate treatments, assessed by stereomicroscopy and ToF‐SIMS.
Journal Article
Improved reverse bias stability in p–i–n perovskite solar cells with optimized hole transport materials and less reactive electrodes
by
Christoforo, M. Greyson
,
Gould, Isaac E.
,
Marder, Seth R.
in
639/301/299
,
639/4077/909/4101/4096/946
,
Bias
2024
As perovskite photovoltaics stride towards commercialization, reverse bias degradation in shaded cells that must current match illuminated cells is a serious challenge. Previous research has emphasized the role of iodide and silver oxidation, and the role of hole tunnelling from the electron-transport layer into the perovskite to enable the flow of current under reverse bias in causing degradation. Here we show that device architecture engineering has a significant impact on the reverse bias behaviour of perovskite solar cells. By implementing both a ~35-nm-thick conjugated polymer hole transport layer and a more electrochemically stable back electrode, we demonstrate average breakdown voltages exceeding −15 V, comparable to those of silicon cells. Our strategy for increasing the breakdown voltage reduces the number of bypass diodes needed to protect a solar module that is partially shaded, which has been proven to be an effective strategy for silicon solar panels.
Perovskite solar cells degrade when subjected to reverse bias. Jiang et al. show that relatively thick hole transport layers and metal back contacts with improved electrochemical stability afford better tolerance to reverse bias.
Journal Article
The Effect of a Low Degree of Fluorine Substitution on Cotton Fiber Properties
Front Cover: The cover page of article 2300337 by Filipe Natalio and co‐workers shows the chemosynthesis of a glucose derivative depicted in the upper part of the illustration. This last compound is fed to a floating cotton ovule in vitro culture (central illustration), becoming integrated into the fibers (blue dots). These modified fibers show increased mechanical properties, as depicted with the clamps in the lower part of the illustration.
Journal Article
Latest applications of ToF-SIMS characterization for next-generation electronic materials
by
Yao, Yan
,
Lou, Jun
,
Mohite, Aditya
in
Analytical Sciences Symposia
,
Electronic materials
,
On Demand - Surface and Subsurface Microscopy and Microanalysis of Physical and Biological Specimens
2022
Journal Article
Screening hydrogels for antifibrotic properties by implanting cellularly barcoded alginates in mice and a non-human primate
2023
Screening implantable biomaterials for antifibrotic properties is constrained by the need for in vivo testing. Here we show that the throughput of in vivo screening can be increased by cellularly barcoding a chemically modified combinatorial library of hydrogel formulations. The method involves the implantation of a mixture of alginate formulations, each barcoded with human umbilical vein endothelial cells from different donors, and the association of the identity and performance of each formulation by genotyping single nucleotide polymorphisms of the cells via next-generation sequencing. We used the method to screen 20 alginate formulations in a single mouse and 100 alginate formulations in a single non-human primate, and identified three lead hydrogel formulations with antifibrotic properties. Encapsulating human islets with one of the formulations led to long-term glycaemic control in a mouse model of diabetes, and coating medical-grade catheters with the other two formulations prevented fibrotic overgrowth. High-throughput screening of barcoded biomaterials in vivo may help identify formulations that enhance the long-term performance of medical devices and of biomaterial-encapsulated therapeutic cells.
The throughput of the in vivo screening of hydrogels for antifibrotic properties can be increased by tagging the biomaterials with cells and reading their genotype via next-generation sequencing.
Journal Article
Room-Temperature High-Purity Single Photon Emission from Carbon-Doped Boron Nitride Thin Films
2025
Hexagonal boron nitride (hBN) has emerged as an excellent host material for generating room temperature single photons exhibiting high brightness and spin-photon entanglement. However, challenges in improving purity, stability, and scalability limit its use in quantum technologies. Here, we demonstrate highly pure and stable single photon emitters (SPEs) in hBN by directly growing carbon-doped, centimeter-scale hBN thin films using the pulsed laser deposition (PLD) method. These SPEs exhibit room temperature operation with polarized emission, achieving a g(2)(0) value of 0.015, which is among the lowest reported for room temperature SPEs and the lowest achieved for hBN SPEs. It also exhibits high brightness ( around 0.5 million counts per second), remarkable stability during continuous operation (> 15 minutes), and a Debye-Waller factor of 45%. First-principles calculations reveal unique carbon defects responsible for these properties, enabled by PLD's low-temperature synthesis and in-situ doping. Our results demonstrate an effective method for large-scale production of high-purity, stable SPEs in hBN, enabling robust quantum optical sources for various applications.