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Solid-supported polymer-lipid hybrid membrane for bioelectrochemistry of a membrane redox enzyme. 用于膜氧化还原酶生物电化学的固体支撑聚合物-脂质混合膜。
Pub Date : 2025-02-11 DOI: 10.1039/d4lf00362d
Rosa Catania, George R Heath, Michael Rappolt, Stephen P Muench, Paul A Beales, Lars J C Jeuken

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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引用次数: 0
The first year of RSC Applied Interfaces: a retrospective RSC应用接口第一年:回顾
Pub Date : 2025-01-07 DOI: 10.1039/D4LF90034K
Shelley A. Claridge, Jianbin Huang, Serena Margadonna, Ryan Richards and Federico Rosei

A graphical abstract is available for this content

此内容的图形摘要可用
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引用次数: 0
A phosphite derivative with stronger HF elimination ability as an additive for Li-rich based lithium-ion batteries at elevated temperatures† 一种具有较强HF消除能力的亚磷酸酯衍生物,可作为高温富锂基锂离子电池的添加剂
Pub Date : 2024-12-03 DOI: 10.1039/D4LF00326H
Xiangzhen Zheng, Tao Huang, Ying Pan, Yongwei Chen, Mingdeng Wei and Maoxiang Wu

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 Li1.144Ni0.136Co0.136Mn0.544O2 cathode. Further, the comparative evaluation of tris(trimethylsilyl) phosphite (TMSPi), TMSPE, and triethyl phosphite (TEP) as phosphite-based additives for Li1.144Ni0.136Co0.136Mn0.544O2/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 Li1.144Ni0.136Co0.136Mn0.544O2, 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.

亚磷酸酯衍生物作为成膜添加剂可以有效地改善锂离子电池阴极的电化学性能。本文将含有三甲基硅基和乙基官能团的二(三甲基硅基)亚磷酸酯(TMSPE)作为p基添加剂,用于改善Li1.144Ni0.136Co0.136Mn0.544O2阴极的电化学性能。此外,在45℃高压条件下,对三甲基硅基亚磷酸酯(TMSPi)、三甲基硅基亚磷酸酯(TMSPE)和三乙基亚磷酸酯(TEP)作为磷酸基添加剂对Li1.144Ni0.136Co0.136Mn0.544O2/Li电池的性能进行了比较评价。理论计算和表面表征表明,TMSPE在Li1.144Ni0.136Co0.136Mn0.544O2表面形成了更薄、更稳定的阴极电解质界面相(CEI),具有更低的界面阻抗、更强的HF消除能力和对过渡金属溶解的抑制作用,是三种亚磷酸盐基添加剂中电池性能最好的。
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引用次数: 0
Multilevel azopolymer patterning from digital holographic lithography 数字全息光刻的多层偶氮聚合物图案化
Pub Date : 2024-11-26 DOI: 10.1039/D4LF00358F
Marcella Salvatore, Francesco Reda, Fabio Borbone and Stefano Luigi Oscurato

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.

基于偶氮聚合物的无掩模光刻技术可以直接、全光学地制造复杂的表面图案。然而,典型的表面起伏仅限于光滑的轮廓。在这里,通过研究基于计算机生成全息术的全息光刻装置的分辨率、对比度和灰度非线性,我们首次扩展了这种图像化方法来制造具有阶梯状不连续的多层浮雕。
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引用次数: 0
Recycled silicon solar cell-derived nanostructured p-black silicon device for high performance NO2 gas sensor applications† 再生硅太阳能电池衍生的纳米结构p-黑硅器件,用于高性能NO2气体传感器应用†
Pub Date : 2024-11-22 DOI: 10.1039/D4LF00299G
Mahaboobbatcha Aleem, Ramakrishnan Vishnuraj and Biji Pullithadathil

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.

二氧化氮(NO2)是一种有毒气体,可引起呼吸系统问题,感知其存在对环境监测和工业安全至关重要。本研究提出了一种利用部分完成/回收的硅太阳能电池,采用金属辅助蚀刻工艺制造高性能p-黑硅基传感器的新方法来检测NO2气体。利用x射线衍射图、拉曼光谱和横截面FESEM表征进行结构和形态分析,证实了p- b硅传感器的完整性。通过将回收技术与先进的制造方法相结合,所得到的传感器具有出色的灵敏度,低检测限为1ppm,当暴露于浓度为1至5ppm的NO2气体时,响应时间(12 - 14s)快速。灵敏度的提高归因于传感器材料独特的纳米结构梳状形态,这有利于快速电荷传输机制,并且已经提出了一种合理的传感机制,并使用耗尽模型图和能量模型图进行了解释。这种环保和经济的解决方案不仅解决了电子废物问题,而且突出了科学研究中可持续实践的潜力。研究结果强调了环保意识和创新的重要性,展示了气体传感技术的美好未来。通过利用回收材料和先进的制造技术,本研究有助于开发用于环境监测应用的高效、环保传感器,为气体传感器领域的可持续发展和技术先进的未来铺平道路。
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引用次数: 0
Selective separation of Am(iii)/Eu(iii) using heterocyclic bistriazolyl phosphonate grafted zirconia and titania solid phase extractants† 杂环膦酸双三唑接枝氧化锆和氧化钛固相萃取剂†选择性分离Am(iii)/Eu(iii)
Pub Date : 2024-11-21 DOI: 10.1039/D4LF00277F
O.-M. Hiltunen, T. Suominen, J. Aho, M. Otaki, A. Zupanc, S. Hietala, G. Silvennoinen and R. Koivula

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.

金属氧化物的表面功能化与磷酸单层共价键使得生成强大的杂化材料具有增强的分离性能。介孔晶体氧化锆和二氧化钛具有较高的热稳定性和抗氧化、抗酸性和抗辐射分解性,是适用的无机载体。我们制备了选择性固相萃取剂,通过直接将氧化锆和氧化钛表面与N-和s-供体络合剂(即2,6-双三唑吡啶衍生物)接枝,有效地分离镅和铕。在pH为2的二元溶液中,Am/Eu的分离系数高达13,即使在Eu过量溶液中,Am也优于Eu。这些稳定的混合材料可以用于分离目的,而不会发生实质性的降解,与常用的溶剂萃取方法相比,提供了有利的可重复使用性和更环保的选择。
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引用次数: 0
Electrophoretically deposited artificial cathode electrolyte interphase for improved performance of NMC622 at high voltage operation† 电泳沉积人工阴极电解质界面,用于提高NMC622在高压操作下的性能†
Pub Date : 2024-11-21 DOI: 10.1039/D4LF00319E
Inbar Anconina and Diana Golodnitsky

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 LiNi0.6Mn0.2Co0.2O2 (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.

高压富镍活性材料广泛应用于高能量密度锂离子电池的负极中。然而,高电荷截止电压会导致电解液分解、过渡金属溶解、结构畸变等引起的显著降解和容量衰退。本文在LiNi0.6Mn0.2Co0.2O2 (NMC622)阴极表面制备了一种人造阴极电解质界面相(ART-CEI)作为保护涂层。以银镁石Li6PS5Cl (LPSC)离子导电纳米颗粒和聚合离子液体(PIL)为粘结剂制备复合膜,电泳沉积在阴极表面。我们发现,在高压(4.3和4.5 V)下,涂层改善了容量保持。除了稳定性提高外,涂层阴极的电化学性能还表现出阳极固体电解质界面(SEI)、阴极电解质界面(CEI)和循环过程中电荷转移过程的速率性能提高和电阻降低。
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引用次数: 0
High-efficiency prediction of water adsorption performance of porous adsorbents by lattice grand canonical Monte Carlo molecular simulation† 用晶格大正则蒙特卡罗分子模拟高效预测多孔吸附剂的吸水性能
Pub Date : 2024-11-18 DOI: 10.1039/D4LF00354C
Zhilu Liu, Wei Li and Song Li

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.

水吸附因其在环境和能源相关领域的巨大应用潜力而备受关注。考虑到广阔的吸附剂空间,计算研究在促进潜在候选物的发现方面起着至关重要的作用。然而,由于计算时间和费用的限制,利用传统的大规范蒙特卡罗(GCMC)来确定最佳吸附剂的大规模计算部署是具有挑战性的。本文采用原子势驱动的主-客体和客体-客体相互作用分层构建的晶格GCMC方法(LGCMC),利用粗粒度Molinero水(mW)模型,准确、快速地模拟了吸附剂的吸附性能。然而,考虑到mW模型的单原子性质,导致纳米尺度约束下不同的相行为,与实验相比,原始lgcmc预测的等温线存在显着差异,特别是不同的阶跃位置。因此,采用调整饱和压力的一般吸附等温线校正策略。以金属-有机骨架(MOFs)为例,采用LGCMC校正策略,得到了与实验结果一致的模拟水吸附等温线。值得强调的是,用LGCMC模拟吸附剂中的水吸附可以在几个小时内完成,与传统的GCMC模拟相比,这产生了两到三个数量级的显著加速。因此,修正后的LGCMC是筛选大量吸附剂的有力工具,有助于发现与水吸附相关的潜在吸附剂,本研究为多孔吸附剂的水吸附机制提供了微观见解。
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引用次数: 0
A diatom frustule-based Mn2SiO4@C@SiO2 multilayer-structure composite as a high-performance anode electrode material for lithium-ion batteries† 基于硅藻支架Mn2SiO4@C@SiO2多层结构复合材料作为高性能锂离子电池负极材料†
Pub Date : 2024-11-18 DOI: 10.1039/D4LF00324A
Shimao Sun, Hongchang Liu, Yuxin Chen, Hongwei Liu, Rongda Yu, Xingfu Zheng, Yunchao Li, Jian Zhu, Jinlan Xia and Jun Wang

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.

二氧化硅储量丰富,理论比容量高,已作为锂离子电池的负极材料进行了测试。然而,它的利用受到循环过程中体积膨胀和低导电性的限制。大多数研究都集中在设计SiO2纳米结构或将其与导电相结合来解决这一问题。本研究以具有天然中空多孔结构的硅藻基生物二氧化硅为模板,通过水热法制备了包覆Mn2SiO4纳米团簇的硅藻基二氧化硅阳极材料。得到了结构为Mn2SiO4@C@SiO2的复合材料。电化学还原过程中生成的Mn/SiO2@C@SiO2夹层结构具有高容量和优异的速率性能,显著抑制了SiO2的体积膨胀。制备的Mn/SiO2@C@SiO2结构的负极材料(AFD@C-Mn-40)在100 mA g - 1下循环100次后仍保持约1112 mA h g - 1的放电比容量,为二氧化硅的大规模应用提供了新的前景。
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引用次数: 0
Analysis of interactions between amino acids and monolayers of charged side chains† 氨基酸与带电荷侧链单层之间相互作用的分析
Pub Date : 2024-11-18 DOI: 10.1039/D4LF00310A
Akira Nomoto, Kentaro Shiraki and Tsukuru Minamiki

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.

蛋白质-蛋白质相互作用(PPIs)是由氨基酸之间的多种相互作用调节的。然而,由于难以分析氨基酸之间的弱相互作用和非特异性相互作用,目前尚不清楚单个氨基酸-氨基酸相互作用(AAIs)在ppi中的作用。因此,我们构建了一个定量分析模型,使用自组装单层(SAMs)装置来评估AAIs。我们可以根据电响应来计算氨基酸与氨基酸侧链之间的μ m级解离常数。在阳离子氨基酸组中,在带负电荷的SAM(3-巯基丙酸)上观察到浓度依赖性反应。这些反应受到竞争离子的浓度和价态的调节,这表明氨基酸之间的静电相互作用强度是不同的。相比之下,本研究中使用的所有氨基酸的非特异性反应都是在带正电的SAM(2-巯基乙胺)上获得的。这些结果表明,相互作用的选择性取决于组装态侧链的类型。我们认为,本研究构建的分析平台可以用于评估控制ppi的各种aai。
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引用次数: 0
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