Mesoporous silica functionalized with an AIE luminogen for drug delivery

An aggregation-induced emission (AIE) luminogen, tetraphenylethene, has been successfully grafted onto mesoporous silica SBA-15 for the first time. The materials emit blue light upon UV irradiation, and are photostable for the ibuprofen (IBU) drug loading and release process, indicating their great potential for biomedical applications.     

基于法布里-珀罗标准具的532 nm多普勒测风激光雷达系统设计和分析

 设计了采用532 nm 种子注入稳频钇铝石榴石（YAG）激光器作为辐射源的基于四通道法布里-珀罗标准具的瑞利和米散射测风激光雷达系统。介绍了激光雷达的多普勒测量基本原理;给出了雷达系统的主要参数,重点对基于分子后向散射信号的外侧双通道标准具的带宽、自由谱间距、峰值间距等指标进行了详细设计与分析,确定了内侧双通道标准具参数;对全系统速度灵敏度、信噪比与探测距离的关系进行了理论模拟。结果表明,可以实现从边界层至对流层高低空一体化探测。     

Chemical-Mechanical Robustness of Single-Crystalline Ni-Rich Cathode Enabled by Surface Atomic Arrangement Control

Layered transition metal oxide cathodes have been one of the dominant cathodes for lithium-ion batteries with efficient Li⁺ intercalation chemistry. However, limited by the weak layered interaction and unstable surface, mechanical and chemical failure plagues their electrochemical performance, especially for Ni-rich cathodes. Here, adopting a simultaneous elemental-structural atomic arrangement control based on the intrinsic Ni−Co−Mn system, the surface role is intensively investigated. Within the invariant oxygen sublattice of the crystal, a robust surface with the synergistic concentration gradient and layered-spinel intertwined structure is constructed on the model single-crystalline Ni-rich cathode. With mechanical strain dissipation and chemical erosion suppression, the cathode exhibits an impressive capacity retention of 82 % even at the harsh 60 °C after 150 cycles at 1 C. This work highlights the coupling effect of structure and composition on the chemical-mechanical properties, and the concept will spur more researches on the cathodes that share the same sublattice.     

Layer-by-layer assembled microgel films with high loading capacity: reversible loading and release of dyes and nanoparticles

Multilayer films containing microgels of chemically cross-linked poly(allylamine hydrochloride) (PAH) and dextran (named PAH-D) were fabricated by layer-by-layer deposition of PAH-D and poly(styrene sulfonate) (PSS). The successful fabrication of PAH-D/PSS multilayer films was verified by quartz crystal microbalance measurements and cross-sectional scanning electron microscopy. The as-prepared PAH-D/PSS multilayer films can reversibly load and release negatively charged dyes such as methyl orange (MO) and fluorescein sodium and mercaptoacetic acid-stabilized CdTe nanoparticles. The loading capacity of the film for MO can be as large as approximately 3.0 microg/cm2 per bilayer, which corresponds to a MO density of 0.75 g/cm3 in the film. The high loading capacity of the PAH-D/PSS films originates from the cross-linked film structure with sufficient binding groups of protonated amine groups, as well as their high swelling capability by solvent. The loaded material can be released slowly when immersing the films in 0.9% normal saline. Meanwhile, the PAH-D/PSS multilayer films could deposit directly on either hydrophilic or hydrophobic substrates such as quartz, polytetrafluoroethylene, polystyrene, poly(ethylene terephthalate), and polypropylene. The microgel films of PAH-D/PSS are expected to be widely useful as matrixes for loading functional guest materials and even for controlled release.     

激光产生温稠密物质的微观动力学过程及状态诊断

随着大型激光装置的建立和精密测量技术的发展,强激光与固体相互作用成为实验室产生温稠密物质的一个重要手段。温稠密物质的结构复杂性、瞬态性和非平衡性给理论建模和实验测量带来了巨大挑战。本文系统介绍了激光产生温稠密物质的实验手段和理论模拟方法方面的重要进展,分析了其中的电子激发动力学、电子-离子能量弛豫过程、离子动力学等物理过程,总结了温稠密物质状态诊断的实验技术和理论方法,并论述了激光产生温稠密物质的发展趋势。     

Multipolar Porphyrin-Triazatruxene Arrays for Two-Photon Fluorescence Cell Imaging

Two-photon excited fluorescent (TPEF) materials are highly desirable for bioimaging applications owing to their unique characteristics of deep-tissue penetration and high spatiotemporal resolution. Herein, by connecting one, two, or three electron-deficient zinc porphyrin units to an electron-rich triazatruxene core via ethynyl π-bridges, conjugated multipolar molecules TAT-(ZnP) _n (n=1–3) were developed as TPEF materials for cell imaging. The three new dyes present high fluorescence quantum yields (0.40–0.47) and rationally improved two-photon absorption (TPA) properties. In particular, the peak TPA cross section of TAT-ZnP (436 GM) is significantly larger than that of the ZnP reference (59 GM). The δ_TPA values of TAT-(ZnP)₂ and TAT-(ZnP)₃ further increase to 1031 and up to 1496 GM, respectively, indicating the effect of incorporated ZnP units on the TPA properties. The substantial improvement of the TPEF properties is attributed to the formation of π-conjugated quadrapole/octupole molecules and the extension of D -π-A-D systems, which has been rationalized by density function theory (DFT) calculations. Moreover, all of the three new dyes display good biocompatibility and preferential targeting ability toward cytomembrane, thus can be superior candidates for TPEF imaging of living cells. Overall, this work demonstrated a promising strategy for the development of porphyrin-based TPEF materials by the construction and extension of D -π-A-D multipolar array.     

Preferential Cation Vacancies in Perovskite Hydroxide for the Oxygen Evolution Reaction

The oxygen evolution reaction (OER) is an ideal model to study the relationship between the activity and the surface properties of catalysts. Defect engineering has been extensively developed to tune the electrocatalytic activity for OER. Compared to the anion vacancies in metal oxides, cation vacancies are more challenging to selectively generate, and the insight into the structure and activity of cation vacancies‐rich catalysts are lacked. Herein, using SnCoFe perovskite hydroxide as a precursor, abundant Sn vacancies on the surface were preferentially produced by Ar plasma. Sn vacancies could be preferentially produced as confirmed by the X‐ray absorption spectra, probably owing to the lower lattice energy and weaker chemical bonds of Sn(OH)₄. The Sn vacancies promoted the exposure of active CoFe sites, resulting in an amorphous surface layer, modulated the conductivity, and thus enhanced the OER performance.     

Biomimetic nanochannels for the discrimination of sialylated glycans via a tug-of-war between glycan binding and polymer shrinkage

Sialylated glycans that are attached to cell surface mediate diverse cellular processes such as immune responses, pathogen binding, and cancer progression. Precise determination of sialylated glycans, particularly their linkage isomers that can trigger distinct biological events and are indicative of different cancer types, remains a challenge, due to their complicated composition and limited structural differences. Here, we present a biomimetic nanochannels system integrated with the responsive polymer polyethyleneimine-g-glucopyranoside (Glc-PEI) to solve this problem. By using a dramatic “OFF–ON” change in ion flux, the nanochannels system achieves specific recognition for N-acetylneuraminic acid (Neu5Ac, the predominant form of sialic acid) from various monosaccharides and sialic acid species. Importantly, different “OFF–ON” ratios of the conical nanochannels system allows the precise and sensitive discrimination of sialylated glycan linkage isomers, α2–3 and α2–6 linkage (the corresponding ion conductance increase ratios are 96.2% and 264%, respectively). Analyses revealed an unusual tug-of-war mechanism between polymer-glycan binding and polymer shrinkage. The low binding affinity of Glc-PEI for the α2–6-linked glycan caused considerable shrinkage of Glc-PEI layer, but the high affinity for the α2–3-linked glycan resulted in only a slight shrinkage. This competition mechanism provides a simple and versatile materials design principle for recognition or sensing systems that involve negatively charged target biomolecules. Furthermore, this work broadens the application of nanochannel systems in bioanalysis and biosensing, and opens a new route to glycan analysis that could help to uncover the mysterious and wonderful glycoworld.

A glycan-responsive polymer-modified nanochannels system enables the precise discrimination of sialylated glycan linkage isomers via the different “OFF–ON” changes resulting from a “tug-of-war” between polymer-glycan binding and polymer shrinkage.