Stabilizing Liquids Using Interfacial Supramolecular Assemblies

Stabilizing liquids based on supramolecular assembly (non-covalent intermolecular interactions) has attracted significant interest, due to the increasing demand for soft, liquid-based devices where the shape of the liquid is far from the equilibrium spherical shape. The components comprising these interfacial assemblies must have sufficient binding energies to the interface to prevent their ejection from the interface when the assemblies are compressed. Here, we highlight recent advances in structuring liquids based on non-covalent intermolecular interactions. We describe some of the progress made that reveals structure–property relationships. In addition to treating advances, we discuss some of the limitations and provide a perspective on future directions to inspire further studies on structured liquids based on supramolecular assembly.     

Unraveling the Solvent Effect on Solid-Electrolyte Interphase Formation for Sodium Metal Batteries

Ether-based electrolytes are considered as an ideal electrolyte system for sodium metal batteries (SMBs) due to their superior compatibility with the sodium metal anode (SMA). However, the selection principle of ether solvents and the impact on solid electrolyte interphase formation are still unclear. Herein, we systematically compare the chain ether-based electrolyte and understand the relationship between the solvation structure and the interphasial properties. The linear ether solvent molecules with different terminal group lengths demonstrate remarkably distinct solvation effects, thus leading to different electrochemical performance as well as deposition morphologies for SMBs. Computational calculations and comprehensive characterizations indicate that the terminal group length significantly regulates the electrolyte solvation structure and consequently influences the interfacial reaction mechanism of electrolytes on SMA. Cryogenic electron microscopy clearly reveals the difference in solid electrolyte interphase in various ether-based electrolytes. As a result, the 1,2-diethoxyethane-based electrolyte enables a high Coulombic efficiency of 99.9 %, which also realizes the stable cycling of Na||Na₃V₂(PO₄)₃ full cell with a mass loading of ≈9 mg cm⁻² over 500 cycles.     

Carbon Quantum Dots with Near-Unity Quantum Yield Bandgap Emission for Electroluminescent Light-Emitting Diodes

Carbon quantum dots (CQDs) feature bright and tunable photoluminescence, solution processability, and low toxicity, showing great potential in optoelectronics. However, the large-scale synthesis of CQDs with near-unity photoluminescence quantum yield (PLQY) has not been achieved so far. In this study, we perform radical-assisted synthesis of hexagon-shaped CQDs (H-CQDs) delivering near-unity PLQY (96 %). Experimental and theoretical analyses revealed that the large vertically oriented transition dipole moment of H-CQDs originating from high symmetry results in nearly 100 % PLQY. The H-CQDs also exhibited a high electron mobility of up to 0.07 cm² V⁻¹ s⁻¹. These properties enable the H-CQD-based light-emitting diodes with a high external quantum efficiency of 4.6 % and a record maximum brightness of over 11 000 cd m⁻². This study represents a significant advance that CQDs-based electroluminescent device can be utilized for potential display and lighting applications.     

二维电子光谱仪器研制与指标分析

介绍了一种利用光栅分光,光子回波矩阵构型的二维光谱实验装置．利用快速,高灵敏度的EMCCD对信号进行外差单脉冲测量．并对仪器的指标进行了检测,30 min内12路相干光的相位抖动均方差达到λ/200,19 min内染料IR140溶液外差回波信号的稳定性达到λ/90,通过移动平移台测量了仪器的光谱准确性,相移偏差均方差为λ/90,对平移台移动不均匀导致的光谱失真进行了数值模拟．另外在位相调整时为解决样品泵浦探测信号有干涉的问题,提出了相位移动的方法．将散射信号扣除,大大提高了位相调整的准确性．对染料IR144溶液,光合蛋白色素复合体B820的测量与文献一致．     

金纳米粒子降低吸附态细菌叶绿素a荧光量子效率的机理研究

本文通过比较细菌叶绿素a(BChl a)吸附于Au纳米颗粒表面前后吸收光谱、荧光光谱、绝对量子产率和荧光寿命的变化,研究金纳米颗粒表面对吸附态细菌叶绿素a(BChl a)自发荧光辐射过程的影响。结果表明,BChl a吸附到Au纳米颗粒表面后,单体和二聚体BChl a吸收峰位均红移约3nm;BChl a单体发射的荧光峰位置从784nm红移到791nm,BChl a二聚体发射的荧光峰位置从684nm红移到689nm,二者荧光均发生淬灭;荧光量子效率降低;荧光寿命在误差范围内保持不变。原因可能来自两个方面:(1)BChl a吸附到Au导电表面后使得与自发辐射跃迁速率相关的光子能态密度变小,从而使BChl a自发辐射速率降低;(2)BChl a与纳米Au颗粒表面间的无辐射能量转移导致吸附态BChl a非辐射速率增大。     

Multishelled Metal Oxide Hollow Spheres: Easy Synthesis and Formation Mechanism

Uniform multishelled NiO, Co₃O₄, ZnO, and Au@NiO hollow spheres were synthesized (NiO and Co₃O₄ hollow spheres for the first time) by a simple shell‐by‐shell self‐assembly allowing for tuning of the the size, thickness and shell numbers by controlling the heat treatment, glucose/metal salt molar ratio, and hydrothermal reaction time. These findings further the development of synthetic methodologies for multishelled hollow structures and could open up new opportunities for deeper understanding of the mechanisms of shell‐by‐shell self‐assembly. Moreover, the double‐shelled NiO hollow sphere exhibits a higher photocatalytic activity for degradation of methyl orange than its morphological counterparts.     

Recording ion channels across soy-extracted lecithin bilayer generated by water-soluble quantum dots

We report on the quantum dot (QD)-induced ion channels across a soya-derived lecithin bilayer supported on a laser drilled of ~100 μm aperture of cellulose acetate substrate that separates two electrolytic chambers. Adequate current bursts were observed when the bilayer was subjected to a gating voltage. The voltage-dependent current fluctuation, across the bilayer, was attributed to the insertion of ~20?nm sized water-soluble CdSe QDs, forming nanopores due to their spontaneous aggregation. Apart from a closed state, the first observable conductance levels were found as 6.3 and 11?nS, as for the respective biasing voltages of ?10 and ?20?mV. The highest observable conductance states, at corresponding voltages were ~14.3 and 21.1?nS. Considering two simplified models, we predict that the non-spherical pores (d_nspore) can be a better approximation over spherical nanopores (d_spore) for exhibiting a definite conductance level. At times, even d_nspore?≤?4d_spore and that the non-spherical nanopores were associated with a smaller No. of QDs than the case for spherical nanopores, for a definite conductance state. It seems like the current events are partly stochastic, possibly due to thermal effects on the aggregated QDs that would form nanopores. The dwell time of the states was predicted in the range of 384–411?μs. The ion channel mechanism in natural phospholipid bilayers over artificial ones will provide a closer account to understand ion transport mechanism in live cells and signaling activity including labelling with fluorescent QDs.     

用荧光显微示踪方法研究RecA在DNA同源识别过程中的工作机理

RecA是原核生物体内参与DNA同源识别过程的一种关键蛋白,长期以来一直是同源重组相关课题的重要研宄对象.通过荧光显微示踪方法,发现在同源识别过程中RecA与单链DNA形成的核蛋白丝与模板DNA的结合是短时(τ=0.2 s)和短程(l=1.05μm)的,结合后搜寻模板DNA上的同源位点的过程可分为布朗运动和定向运动两种模式.结合时核蛋白丝并不是缠绕在模板DNA上,而是以一种更弱的方式结合在模板DNA外侧进行位点搜寻.如果在该过程中没有找到同源位点,核蛋白丝就会脱离模板DNA,并寻找下一次与模板DNA结合的机会,重复以上过程.     

Numerical-experimental hybrid method for stress separation in digital gradient sensing method

A numerical-experimental hybrid method for the stress separation in the digital gradient sensing (DGS) method is proposed in this study. In the proposed hybrid method, boundary conditions for a local finite element model, that is, nodal force along boundaries are inversely determined from experimental values obtained by the digital gradient sensing method. The hybrid method follows two stages. In stage 1, the DGS method measures the Cartesian stress gradient components directly and, subsequently, the sum in Cartesian stresses at all interesting points on the surface; stress sum are used to compute the unknown boundary conditions for the local model. In stage 2, the individual stress components are calculated by the direct finite element method using the computed boundary conditions from stage 1. The effectiveness is demonstrated by applying the proposed method to a stress concentration problem involving concentrated load acting on an edge of a large planar sheet. The individual stress components thus determined are summed and compared with analytical stress sum, confirming the effectiveness and accuracy of the proposed technique.