A Highly Efficient All-Solid-State Lithium/Electrolyte Interface Induced by an Energetic Reaction

The energetic chemical reaction between Zn(NO₃)₂ and Li is used to create a solid-state interface between Li metal and Li_6.4La₃Zr_1.4Ta_0.6O₁₂ (LLZTO) electrolyte. This interlayer, composed of Zn, ZnLi_x alloy, Li₃N, Li₂O, and other species, possesses strong affinities with both Li metal and LLZTO and affords highly efficient conductive pathways for Li⁺ transport through the interface. The unique structure and properties of the interlayer lead to Li metal anodes with longer cycle life, higher efficiency, and better safety compared to the current best Li metal electrodes operating in liquid electrolytes while retaining comparable capacity, rate, and overpotential. All-solid-state Li||Li cells can operate at very demanding current–capacity conditions of 4 mA cm⁻²–8 mAh cm⁻². Thousands of hours of continuous cycling are achieved at Coulombic efficiency >99.5 % without dendrite formation or side reactions with the electrolyte.     

氧化石墨烯的表面化学修饰及纳米-生物界面作用机理

由于具备独特的物理化学性质,氧化石墨烯已被广泛地应用于生命科学与人体健康等相关领域.然而,如何最大化地发挥氧化石墨烯的优势与特点,并克服其自身固有性质导致的生物不良效应,依然是当前面临的难题.为更好地了解该领域的研究现状,本文主要综述了近年来氧化石墨烯的表面化学调控和生物作用机理方面的最新研究进展.首先,简要介绍了氧化石墨烯的物理化学特性、典型的表面化学调控策略(氧化还原、羧基化、氨基化、有机小分子修饰、聚合物修饰、多肽/蛋白修饰、核酸修饰和纳米颗粒修饰),以及不同表面修饰引起的生物效应.继而,重点总结了氧化石墨烯表面修饰影响其生物效应的主要界面作用机理,包括蛋白冠形成、细胞膜损伤、膜受体作用与氧化应激损伤.最后,针对氧化石墨烯表面化学调控和生物效应与机理相关研究所面临的科学问题与挑战进行了展望.     

Interfacial Design of Dendrite-Free Zinc Anodes for Aqueous Zinc-Ion Batteries

Aqueous zinc-ion batteries have rapidly developed recently as promising energy storage devices in large-scale energy storage systems owing to their low cost and high safety. Research on suppressing zinc dendrite growth has meanwhile attracted widespread attention to improve the lifespan and reversibility of batteries. Herein, design methods for dendrite-free zinc anodes and their internal mechanisms are reviewed from the perspective of optimizing the host–zinc interface and the zinc–electrolyte interface. Furthermore, a design strategy is proposed to homogenize zinc deposition by regulating the interfacial electric field and ion distribution during zinc nucleation and growth. This Minireview can offer potential directions for the rational design of dendrite-free zinc anodes employed in aqueous zinc-ion batteries.     

Atomic‐Scale Insight into Exsolution of CoFe Alloy Nanoparticles in La0.4Sr0.6Co0.2Fe0.7Mo0.1O3−δ with Efficient CO2 Electrolysis

In situ exsolution of metal nanoparticles in perovskite under reducing atmosphere is employed to generate a highly active metal–oxide interface for CO₂ electrolysis in a solid oxide electrolysis cell. Atomic‐scale insight is provided into the exsolution of CoFe alloy nanoparticles in La_0.4Sr_0.6Co_0.2Fe_0.7Mo_0.1O_3?δ (LSCFM) by in situ scanning transmission electron microscopy (STEM) with energy‐dispersive X‐ray spectroscopy and DFT calculations. The doped Mo atoms occupy B sites of LSCFM, which increases the segregation energy of Co and Fe ions at B sites and improves the structural stability of LSCFM under a reducing atmosphere. In situ STEM measurements visualized sequential exsolution of Co and Fe ions, formation of CoFe alloy nanoparticles, and reversible exsolution and dissolution of CoFe alloy nanoparticles in LSCFM. The metal–oxide interface improves CO₂ adsorption and activation, showing a higher CO₂ electrolysis performance than the LSCFM counterparts.     

可用于活细胞线粒体随机光学重构超分辨成像的分子内可逆环化五甲川菁染料探针

基于单分子定位的随机光学重构超分辨成像作为一种先进的光学成像方法,可用于尺寸小于光学衍射极限的生物结构的超清晰成像,为在单分子层面研究疾病的发病机制及寻找精准的治疗策略提供有力研究工具,在生物医学领域有着广泛的应用前景.随机光学重构超分辨成像技术依赖于标记探针的光物理性质,探针需要在大量缓冲试剂及含巯基试剂存在下才能产生稳定光致闪烁进行超分辨成像,获得理想的超分辨成像结果,但是大量缓冲试剂与巯基试剂对活细胞伤害较大,使得其在活细胞的超分辨成像应用上存在困难,而限制了其在生物医学成像领域的进一步应用,因此,需要开发可用于活细胞的单分子定位超分辨成像的新型光学探针.本工作提出了一种新的可用于单分子定位超分辨成像的五甲川菁染料探针,不需要外加成像缓冲液及巯基试剂就可以产生光致闪烁变化.基于此,开发了一种分子内自发开、关环反应的新型五甲川菁染料探针,具有活细胞膜通透性.探针不需要使用缓冲液体系及对细胞有害的含巯基试剂,在低功率单束激光直接照射下产生光致闪烁,探针对活细胞没有产生明显毒性,适合活细胞的超分辨成像.进入活细胞后探针选择性定位于细胞线粒体上,在激光照射下产生光致闪烁,电子倍增电荷耦合...     

真空溶剂蒸发全二维液相色谱接口及其应用

以正相色谱(NPLC)为第一维,反相色谱(RPLC)为第二维,建立了真空溶剂蒸发接口的全二维液相色谱系统(VEI-C2DLC)。样品首先在第一维(CN色谱柱)进行正相分离,第一维洗脱产物被交替存储到十通阀上的两个定量环中,与此同时对切割到定量环内的第一维组分进行在线真空蒸发,被分析样品组分保留在定量环内壁内,而溶剂被蒸发除去。十通阀切换后保留在该定量环内的样品组分被洗脱到第二维进行反相分离,如此反复循环使第一维组分完全转移到第二维。采用标准样品和天然植物蛇床子提取液对该全二维液相系统进行了评价。     

Anionic behavior and single-molecule crystal in fullerene confinements: A contribution from DFT energy decomposition and cooperativity analyses

The recently proposed systems of various anions (A) confined inside C₆₀ , A⁻ @ C₆₀ , which in turn behave as large and stable anions, (A @ C₆₀)⁻ , can find potential applications in various fields. On the other hand, it has earlier been shown that from the dihalogens (X₂ ) encapsulated C₆₀ , X₂ @ C₆₀ , only F₂ @ C₆₀ can be introduced as a system in which the cage acts as a cation C₆₀⁺ and interacts with an endohedral anion, F₂⁻ , forming the F₂⁻ @ C₆₀⁺ as a single-molecule crystal compound. In this work, two density functional theory energy decomposition analysis (EDA) schemes, where in one of them the noninteracting kinetic, electrostatic, and exchange-correlation energies come into play while another scheme, called as EDA-SBL, includes the steric, electrostatic, and quantum effects as essential ingredients (S. Liu, J. Chem. Phys. 2007 , 126, 244103), are utilized to find out what energetic components govern the unique characteristics of the (A @ C₆₀)⁻ and X₂ @ C₆₀ confinements. It is shown that the noninteracting kinetic energy and steric energies have important contributions to the total interaction energies for the considered systems. However, there are other confinements for which the electrostatic and exchange-correlation contributions play also imperative roles. Furthermore, we find reasonable correlations between interaction energies and their components as well as the energetic components themselves, leading to an alternative EDA scheme including the noninteracting kinetic, steric, and electrostatic energies for investigations on other endohedral fullerenes. Extending our analyses to large size confinements, Cl⁻ @ C_n with n up to 90 as illustrative examples, the quantitative cooperativity concept is also explored, where the positive and negative cooperativity profiles unveil a specific size of the anionic confinements to form the most stable large anion.     

Al2O3-CeO2复合电解质的制备及其半导体离子燃料电池性能

通过共沉淀法制备了Al₂O₃-CeO₂复合材料,并将其作为电解质应用于半导体离子燃料电池（SIFC）。探究了Al₂O₃、CeO₂物质的量之比不同的Al₂O₃-CeO₂复合电解质对SIFC电化学性能的影响。采用X射线衍射（XRD）、X射线光电子能谱（XPS）、扫描电子显微镜（SEM）和透射电子显微镜（TEM）对材料进行了表征。其中,Al₂O₃、CeO₂物质的量之比为1：0.5的Al₂O₃-CeO₂（1：0.5）电池获得了最佳性能,在550℃下,开路电压为1.099 V时最大功率密度为1 142 mW·cm^-2。得益于复合电解质在测试气氛下两相间的界面效应,Al₂O₃-CeO₂（1：0.5）电池在较低测试温度下取得了优异的混合离子传导和功率输出性能。     

Chirality Discrimination at Binary Organic|Water Interfaces Monitored by Interfacial Tension Measurements with Preliminary Comparison with Molecular Dynamics Simulations

Chirality discrimination at a binary toluene (organic)/water(aqueous) interface between R- or S-Tol-BINAP (2,2′-Bis(di-p-tolylphosphino)-1,1′-binaphthyl) molecules and the water-soluble serine chiral specie is examined for the first time, using a combination of interfacial tension measurements and molecular dynamic simulations. Experimental interfacial measurements exhibit a clear chirality-controlled difference when a homochiral versus a heterochiral enantiomeric pairs are introduced at the interfaces. The related molecular dynamics simulations support the experimental results and provide further molecular insight of intermolecular interactions at the interfaces. The results indicate that interfacial tension measurements can capture the preferential interactions which exist between different pairs of enantiomers at the binary interfaces, opening up a new way for probing chirality discrimination at liquid-liquid interfaces.