RSC Applied Interfaces最新文献

Hybrid membranes, consisting of phospholipids and amphiphilic block polymers, offer enhanced stability compared to liposomes and greater biocompatibility than polymersomes. These qualities make them a versatile platform for a wide range of applications across various fields. In this study, we have investigated the ability of solid-supported polymer-lipid hybrid membranes (SSHM) to act as a platform for bioelectrochemistry of membrane proteins. The redox enzyme, cytochrome bo ₃ (cyt bo ₃ ), a terminal oxidase in Escherichia coli, was reconstituted into hybrid vesicles (HVs), which were subsequently tested for their ability to form SSHMs on different self-assembled monolayers (SAMs) on gold electrodes. SSHM formation was monitored with electrochemical impedance spectroscopy (EIS), quartz crystal microbalance with dissipation (QCM-D), and atomic force microscopy (AFM). SSHMs were successfully formed on gold electrodes with mixed SAMs of 6-mercapto-1-hexanol and 1-hexanethiol at a 1 : 1 ratio. The activity of cyt bo ₃ was confirmed using cyclic voltammetry (CV), with electron transfer to cyt bo ₃ mediated by a lipophilic substrate-analogue decylubiquinone (DQ). SSHMs formed with HVs-cyt bo ₃ samples, stored for more than one year before use, remain bioelectrocatalytically active, confirming our previously established longevity and stability of HV systems.

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Phosphite derivatives as film forming additives can effectively improve the electrochemical performance of cathodes in Li-ion batteries (LIBs). In this work, ethyl bis(trimethylsilyl) phosphite (TMSPE), which contains trimethylsilyl and ethyl functional groups, is used as a P-based additive for improving the electrochemical performance of a Li_1.144Ni_0.136Co_0.136Mn_0.544O₂ cathode. Further, the comparative evaluation of tris(trimethylsilyl) phosphite (TMSPi), TMSPE, and triethyl phosphite (TEP) as phosphite-based additives for Li_1.144Ni_0.136Co_0.136Mn_0.544O₂/Li cells at 45 °C under a high voltage is also presented. Theoretical calculations and surface characterization revealed that TMSPE formed a thinner and stable cathode electrolyte interphase (CEI) on the surface of Li_1.144Ni_0.136Co_0.136Mn_0.544O₂, which has lower interfacial impedance, stronger HF elimination, and transition metal dissolution inhibition, resulting in the best cell performance among the three phosphite-based additives.

Azopolymer-based maskless lithography enables direct, all-optical fabrication of complex surface patterns. However, typical surface reliefs are limited to smooth profiles. Here, by investigating the resolution, contrast ratio, and gray-scale nonlinearities of a holo-lithographic setup based on computer-generated holography, we extend this patterning approach to fabricate, for the first time, multilevel reliefs with step-like discontinuities.

Nitrogen dioxide (NO₂) is a toxic gas that can cause respiratory problems, and sensing its presence is crucial for environmental monitoring and industrial safety. This investigation presents a novel approach towards sensing NO₂ gas by utilizing partially completed/recycled silicon solar cells employing a metal-assisted etching process to fabricate a high-performance p-black-silicon based sensor. Structural and morphological analyses using X-ray diffraction patterns, Raman spectroscopy and cross sectional FESEM characterization confirm the integrity of the p-B-silicon sensor. By combining recycling techniques with advanced fabrication methods, the resulting sensor exhibits exceptional sensitivity, a low detection limit of 1 ppm, and rapid response times (12–14 s) when exposed to NO₂ gas concentrations ranging from 1 to 5 ppm. The enhanced sensitivity is attributed to the unique nanostructured comb-like morphology of the sensor material, which facilitates fast charge transport mechanisms, and a plausible sensing mechanism has been proposed and explained using a depletion model diagram and energy model diagram. This eco-friendly and cost-effective solution not only addresses electronic waste concerns but also highlights the potential of sustainable practices in scientific research. The findings emphasize on the importance of environmental consciousness and innovation, showcasing a promising future for gas sensing technology. By utilizing recycled materials and advanced fabrication techniques, this study contributes to the development of efficient, eco-friendly sensors for environmental monitoring applications, paving the way for a more sustainable and technologically advanced future in the field of gas sensors.

Surface functionalization of metal oxides with phosphonic acid monolayers by covalent bonding enables the generation of robust hybrid materials with enhanced separation properties. Mesoporous crystalline zirconia and titania serve as applicable inorganic supports with high thermal stability and resistance to oxidation, acidity and radiolysis. We have fabricated selective solid phase extractants that efficiently separate americium and europium from each other, via straightforward grafting of the zirconia and titania surfaces with N- and S-donor complexing agents, namely 2,6-bis-triazolyl-pyridine derivatives. Separation factors (Am/Eu) up to 13 were obtained in binary solution at pH 2 and preference for Am over Eu was observed even in Eu excess solution. These stable hybrid materials can be utilized for separation purposes without substantial degradation, providing advantageous reusability and a greener option in comparison to commonly used solvent extraction methods.

High-voltage Ni-rich active materials are widely used in cathodes of high-energy-density lithium-ion batteries (LIBs). However, the high charge cutoff voltages lead to significant degradation and capacity fading, caused by electrolyte decomposition, transition metal dissolution, structural distortion, and more. Herein, we present an artificial cathode electrolyte interphase (ART-CEI) as a protective coating on the surface of the LiNi_0.6Mn_0.2Co_0.2O₂ (NMC622) cathode. A composite film, prepared from argyrodite Li₆PS₅Cl (LPSC) ion conducting nanoparticles and a polymerized ionic liquid (PIL) as a binder, was electrophoretically deposited on the surface of the cathode. We found that capacity retention at high-voltage operation (4.3 and 4.5 V) is improved due to the coating. Besides the stability improvement, the electrochemical performance of the coated cathode shows an enhancement in rate performance and lower resistances of the anode solid electrolyte interphase (SEI), the cathode electrolyte interphase (CEI), and charge transfer processes during cycling.

Water adsorption has come under the spotlight for its tremendous potential in numerous environment- and energy-related applications. Given the vast adsorbent space, computational studies play a critically significant role in facilitating the discovery of potential candidates. However, large-scale computational deployment by conventional grand canonical Monte Carlo (GCMC) to identify optimal water adsorbents is challenging due to its extreme computation time and expense. In this work, a lattice GCMC method (LGCMC) with hierarchically constructed discretized interaction of host–guest and guest–guest driven by atomistic potentials was attempted to accurately and rapidly simulate the water adsorption performance of adsorbents using a coarse-grained Molinero water (mW) model. Nevertheless, given the monatomic nature of the mW model, leading to different phase behaviors in nanoscale confinement, a remarkable discrepancy in the primitive LGCMC-predicted isotherms, especially different step positions, compared with experiments was observed. Thus, a general correction strategy of water adsorption isotherm by tuning the saturation pressure was adopted. Taking metal–organic frameworks (MOFs) as examples, simulated water adsorption isotherms consistent with experimental results were obtained by the correction strategy using LGCMC. It is worth highlighting that the simulation of water adsorption in adsorbents by LGCMC can be accomplished within a few hours, which yields a significant acceleration of two to three orders of magnitude compared to conventional GCMC simulations. Therefore, the corrected LGCMC is a powerful tool to screen a huge number of adsorbents to facilitate the discovery of potential adsorbents for water adsorption-related applications, and this study provides microscopic insights into water adsorption mechanisms in porous adsorbents.

Owing to its abundant reserves and high theoretical specific capacity, silica has been tested as an anode material for lithium-ion batteries. However, its utilization is limited by volume expansion during cycling and low electrical conductivity. Most studies have focused on designing nanostructures of SiO₂ or combining them with conductive phases to solve this problem. In this work, diatom-based biological silica with a natural hollow porous structure was used as a template to prepare diatom-based silica anode materials coated with Mn₂SiO₄ nanoclusters via a hydrothermal method. A composite material with a structure of Mn₂SiO₄@C@SiO₂ was obtained. The Mn/SiO₂@C@SiO₂ sandwich structure derived during electrochemical reduction has a high capacity and excellent rate performance and significantly inhibits the volume expansion of SiO₂. The prepared anode material (AFD@C-Mn-40) with the Mn/SiO₂@C@SiO₂ structure retained a specific discharge capacity of approximately 1112 mA h g⁻¹ after 100 cycles at 100 mA g⁻¹, which provides new prospects for the large-scale application of silica.

Protein–protein interactions (PPIs) are regulated by multiple interactions among amino acids. However, the contribution of individual amino acid–amino acid interactions (AAIs) in PPIs is currently unclear because it is difficult to analyze the weak and nonspecific interactions among amino acids. Therefore, we constructed a quantitative analytical model to evaluate AAIs using a device with self-assembled monolayers (SAMs). We could evaluate the μM-order dissociation constant between amino acids and the side chain of amino acids based on the electrical response. In the cationic amino acid group, concentration-dependent responses were observed on a negatively charged SAM (3-mercaptopropionic acid). These responses were modulated by the concentration and valence of the competing ions, which indicated that the strength of electrostatic interactions among amino acids is different. In contrast, nonspecific responses to all amino acids used in this study were obtained on a positively charged SAM (2-mercaptoethylamine). These results indicate that the selectivity of interaction depends on the type of side chain in the assembled state. We believe that the analytical platform constructed in this study can be adapted to evaluate various AAIs that govern PPIs.