Advanced Materials Interfaces最新文献

All-solid-state batteries (ASSBs) have gained much interest in recent years because they promise higher energy and power densities as well as improved safety over lithium-ion batteries (LIBs). This is achieved by using non-flammable solid electrolytes (SEs) together with lithium metal or high-capacity silicon anodes. One major hurdle to overcome is the permanent intimate contact of all cell components to enable long-term cycling stability. This study investigates the macroscopic (microstructure) and microscopic (atomistic) effects of uniaxial stack pressure on the transport properties of free-standing, slurry-processed tetragonal $�{\mathrm{Li}}_7$$�{\mathrm{SiPS}}_8$ (t-Li₇SiPS₈) sheets, containing different solid electrolyte (SE)-to-binder ratios (SE:B) and particle size fractions. The results demonstrate that binder content and particle size significantly influence the morphology as evidenced by synchrotron-radiation computed tomography (CT), pressure response, and ionic conductivity of the sheets. Notably, while compression mechanics are consistent across samples, relative densities, and ionic conductivities are more dependent on binder content than particle size. Larger particles and lower binder contents generally led to higher ionic conductivities. The study also reveals that activation volumes appear to increase with binder content, suggesting that extrinsic factors, particularly the binder, may obscure the calculation of the intrinsic activation volumes of t-Li₇SiPS₈. Thus, the obtained values for binder-containing sheets may be considered apparent values. Contrary to expectations, repeated compression cycles led to a decreased ionic conductivity and relative density, likely due to microstructural damage and increased (apparent) activation volumes. Overall, the study serves as a reminder to the community to carefully interpret intrinsic values, such as the activation volume, and by extension the activation energy, in the increasingly popular binder-containing SE sheet systems.

Efficient charge transfer at heterostructure interfaces is crucial for optoelectronic devices. Quasi-2D perovskites with varied layer thicknesses form multiple interfaces, hindering transport. Transient absorption spectroscopy reveals strategic phase distribution enables ultrafast energy transfer across phases and narrow-band emission from high-n phases. Photocurrent and surface potential change indicates directional charge transport exhibits in Quasi-2D perovskites, underscoring the impact of phase distribution on device performance. More details can be found in the Research Article by Sachin R. Rondiya and co-workers (DOI: 10.1002/admi.202500108).

Microscopic carbon/SiO₂ composites are composed of a huge number of interfacial contacts. When those are exposed to moderate ohmic fields gas adsorptivity of the composite is modulated. Herein it shows that it is possible to manipulate, modify, and follow gas adsorption selectivity by in situ spectroscopy under electrical charging. In a model gas mixture of CO₂ and N₂, for the first time it can be shown that a change in gas composition is observed and can be controlled locally above an electrically charged carbon/SiO₂ surface using in situ Raman spectroscopy. The technique is implemented in an ongoing non-stationary adsorption process using the advantage of the fast on-off switchability of the electric field as compared to the typically slow equilibration kinetics of adsorption on activated carbon. An increase in gas phase concentration of 3.5% and 5.5% of CO_2, which is equivalent to a change in selectivity of 11% and 24% of CO₂ over N_2, just by applying an electrical input power of 0.53 and 1.12 W is achieved and quantified by Raman spectroscopy, respectively. The method bears general potential for mixtures of gases with different responses to the electric field, as well as for processes where a local manipulation of gas concentrations is necessary.

Semiconductor thin films are foundational to a broad range of optoelectronic technologies. Solution deposition offers a low-cost, energy-efficient alternative to vapor-based methods, but its practical scalability is hindered by poor reproducibility and high defect densities arising from complex interdependencies among processing variables. Statistical design of experiments (DoE) enables critical insight into the non-intuitive interdependencies that are not accessible by conventional one-variable-at-a-time (OVAT) approaches. Using Sb₂Se₃ as an example semiconductor, DoE is employed with a central composite design (CCD) to systematically vary six processing parameters encompassing ink formulation and deposition parameters. From only 77 experiments, predictive models are constructed for four macro- and microscopic defect types known to interrupt charge transport. All six variables are found to significantly and synergistically influence film quality and are optimized to minimize defect density. Importantly, the optimal film exhibited a threefold enhancement in photoresponse in single-junction devices with no detectable change in composition, nanostructure, or film stability, implicating defect suppression as the critical driver of improved performance. This work highlights DoE as a powerful methodology for uncovering latent structure–processing–property relationships in thin films and provides a general framework for accelerating the development of optoelectronic-grade materials via solution processing.

Silicon-based negative electrodes are essential for next-generation high-capacity Li-ion batteries, with SiO₂ emerging as a promising and sustainable option. However, SiO₂ anodes have limited cycling stability, which can be improved by tailoring the solid electrolyte interphase (SEI) through electrolyte engineering. This study investigates the effects of LiPF₆ and LiFSI electrolyte salts, along with fluoroethylene carbonate (FEC) and vinylene carbonate (VC) additives, on the performance of SiO₂ anodes. Galvanostatic cycling and electrochemical impedance spectroscopy (EIS) are combined with SEI composition analysis using Ar⁺-sputtered X-ray photoelectron spectroscopy and hard X-ray synchrotron photoelectron spectroscopy at different photon energies. The results show that FEC enhances capacity retention, while VC improves long-term stability at the expense of lower initial capacity. No synergistic benefits are observed from combination of both additives. LiFSI-based electrolytes deliver high initial capacities but suffer capacity fade over cycling, whereas additive-free LiPF₆ formulations lead to poor cycling stability due to the formation of a thick and resistive SEI layer. In contrast, LiFSI promotes a thinner and more inorganic-rich SEI. Both FEC and VC lead to the formation of a poly(VC) surface layer that enhances capacity retention. The FEC-derived layer, enriched with LiF and thinner in nature, exhibits improved SEI stability. These findings provide valuable insights for designing electrolytes to improve the cycling performance of SiO₂ anodes.

The underwater functionality of superhydrophobic (SHPo) surfaces relies on the presence of a thin trapped air layer, or plastron, yet maintaining this plastron in uncontrolled environments remains a major challenge. Here, a scalable method is reported to convert SHPo surfaces into Salvinia surfaces by selectively coating polydopamine (PDA) on the top surfaces of microstructures. The success is enabled by identifying and overcoming a previously unrecognized barrier unique to PDA coating on SHPo surfaces. Pressure fluctuation experiments demonstrate that the converted Salvinia surfaces have markedly enhanced plastron stability compared with SHPo counterparts of identical microstructure. Complementary mathematical analysis and numerical simulations establish how micrograting and micropost geometries govern plastron stability, providing a design guideline for SHPo and Salvinia surfaces.

Catheter-associated infections are a major concern in hospitals, leading to both life-threatening for the patients and a high cost for society. The development of a straightforward and industrial route to make an antibacterial catheter is thus worthwhile. This study demonstrates that the use of 2 wt.% of an antibacterial MeI-quaternized poly(butyl methacrylate–block–N,N-dimetylaminoethyl methacrylate) P(BMA-b-DMAEMA) copolymer in combination with 2 wt.% of an antiadhesive poly(butyl methacrylate–block–poly(ethylene glycol) methyl ether methacrylate) P(BMA-b-PEG_xMA) copolymer (with x the molecular weight of the PEG) as additives during the extrusion of the polyurethane matrix is an efficient method to produce antibacterial and antiadhesive PU materials without loss of activity after exposure to biologic media. The addition in the formulation of the antiadhesive copolymers enables protecting the surface from passivation and then to keep the contact possible between the bacteria and the antibacterial material. The antibacterial activity of the materials against E. coli and S. aureus is then preserved even after exposure to albumin, plasma, intralipids, or gastric acids. The prepared biomaterials also present no toxicity and are able to limit E. coli biofilm formation. Based on these results, this methodology can be realistically envisioned to elaborate long-lasting venous or enteral catheters.

Ru₃Sn₇ is experimentally demonstrated as an efficient catalyst, with potential utilization of topological surface states for hydrogen evolution reaction. Despite its promising catalytic performance, the topological nature of Ru₃Sn₇ remains uncertain. Particularly, the bulk-boundary correspondence has not yet been established, hence hindering a rigorous justification of its topologically-protected surface states. In this work, the bulk topology of Ru₃Sn₇ is detailed using first-principles calculations and the topological quantum chemistry formalism. Ru₃Sn₇ turns out to be an enforced semimetal possessing symmetry-protected crossings within a set of bands near the Fermi level, which are enforced and prescribed by the violations of symmetry-prescribed compatibility relations. Moreover, the surface states and the associated origin from the same set of entangled bands are identified, thereby establishing the bulk-boundary correspondence. To evaluate the effects of chemical modifications, the response of topological surface states to various surface terminations, stoichiometry, and oxidation is examined. The surface structures are globally optimized, and the phase diagrams for various experimental conditions are built. It is shown that, due to changes in the local chemical environment, the original surface states are significantly altered. Modified surface bands can be observed near the Fermi level on surface terminations that preserve the C_4v symmetry.

Solutions containing hydrofluoric acid (HF) and bromic acid (HBrO₃) are investigated as nitrogen oxide (NO_x)-free mixtures for wet-chemical etching of (100) silicon wafer surfaces. Isotropic etching behavior with high dissolution rates of up to 10 µm min⁻¹ is observed at room temperature, leading to polished surfaces. Anisotropic etching is observed when bromine (Br₂) is added to HF-HBrO₃ solutions. Therefore, monocrystalline (100) silicon wafer surfaces are covered with random upright pyramids with edge lengths of about 5 µm. The etch rate is strongly dependent on the concentration of HBrO₃. Silicon surfaces are analyzed by scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). The gas phase is analyzed using Raman and infra red (IR) spectroscopy. The oxidation of the silicon surface by bromic acid likely takes place via oxygen insertion into the rearward silicon bonds. During etching, multiple active Br-species are formed which alter the etching behavior.

The efficient and stable capture of cells within microfluidic platforms is essential for cellular biology analyses, offering insights into the heterogeneity of cell properties and cellular processes, for example, among cancer cells. However, conventional microfluidic cell confinement modalities, such as water-in-oil emulsions and microstructure trapping, face inherent limitations in biological applicability and precise control. Here an approach is introduced to confine cells in dead-end microstructures leveraging a dextran concentration gradient. This method allows for the fine-tuned capture of cells, reaching the precision of single-cell culture, as demonstrated for yeast and leukemia cells. By incorporating polyethylene glycol (PEG) solutions, phase separation is induced within the microfluidic environment, encapsulating single cells within dextran droplets. The technique is distinguished by its stability, control, and adaptability, paving a new way for innovations not only in cellular biology, but broadly in chemical and biological applications, including the synthesis of bio-oriented particles, microcarrier production, and advancements in tissue engineering.