Na原子链表面等离激元特性的含时密度泛函研究

本文用含时密度泛函理论研究了线性Na原子链的表面等离激元机理.主要在原子尺度下模拟计算了体系随着原子数增加及原子间距变化的集体激发过程.研究发现线性原子链有一个普遍的特性——存在一个纵模和两个横模.两个横模一般在实验上很难被观测到.纵模随着原子链长度增加,能量红移的同时,该纵模主峰的强度呈线性增长.随着原子个数的增加,端点模式(TE)开始蓝移,能量和偶极强度都逐渐趋向饱和.横模能量被劈裂的原因概括如下:(一)每个位置的电子受到的势不同,在两端的电子受到的势要比在中间的电子受到的势要高,因此两端的电荷积累也比中间多;(二)端点存在悬挂键,所以中间的电子-电子间相互作用与端点的不一样,这两方面又都与原子间距d有关.     

Single-emissive-layer all-perovskite white light-emitting diodes employing segregated mixed halide perovskite crystals

Metal halide perovskites have demonstrated impressive properties for achieving efficient monochromatic light-emitting diodes. However, the development of white perovskite light-emitting diodes (PeLEDs) remains a big challenge. Here, we demonstrate a single-emissive-layer all-perovskite white PeLED using a mixed halide perovskite film as the emissive layer. The perovskite film consists of separated mixed halide perovskite phases with blue and red emissions, which are beneficial for suppressing halide anion exchange and preventing charge transfer. As a result, the white PeLED shows balanced white light emission with Commission Internationale de L''Eclairage coordinates of (0.33, 0.33). In addition, we find that the achievement of white light emission from mixed halide perovskites strongly depends on effective modulation of the halide salt precursors, especially lead bromide and benzamidine hydrochloride in our case. Our work provides very useful guidelines for realizing single-emissive-layer all-perovskite white PeLEDs based on mixed halide perovskites, which will spur the development of high-performance white PeLEDs.

We demonstrated a single-emissive-layer all-perovskite white light-emitting diode based on a mixed halide perovskite film.     

Identifying the viscoelastic properties of soft matter from the indentation response of a hard film-soft substrate system

The indentation technique is widely used in measuring the mechanical properties of soft matter at the microscale or nanoscale,but still faces challenges by these unique properties as well as the consequent strong surface adhesion, including the strong nonlinear effect, unclear judgment of the contact point, difficulties in estimating the contact area, and the risk of the indenter piercing the sample. Here we propose a two-step method to solve these problems: lay a hard film on a soft matter, and obtain the viscoelastic properties of this soft matter through the indentation response of this composite structure. We first establish a theoretical indentation model of the hard film-soft substrate system based on the theory of plates, elastic-viscoelastic correspondence principle and Boltzmann superposition principle. To verify the correctness of this method, we measure the mechanical properties of the methyl vinyl silicone rubber(MVSR) covered by a Cu nanofilm. Finally, we test the effectiveness and error sensitivity of this method with the finite element method(FEM). The results show that our method can accurately measure the mechanical properties of soft matter, while effectively circumventing the problems of the traditional indentation technique.     

四方体MgO的制备及对有机染料的吸附

以六水氯化镁和六次甲基四胺为原料,采用水热法合成四方体MgO,考察其对有机染料甲基橙和亚甲基蓝的吸附行为.通过TGA-DTA、SEM、XRD、N2-sorption和FT-IR等手段表征样品.结果表明,原料浓度、温度和表面活性剂对四方体MgO结构的形成影响较小,而反应时间的延长有助于有序结构的组装.温度170℃、时间24h、MgCl2·6H2O与C6H12N4浓度比为1∶2和表面活性剂PVP是制备四方体MgO的最佳条件.在溶液浓度10mg · L-1的单一吸附实验过程中,四方体MgO对甲基橙和亚甲基蓝的去除率分别为91.3;和22.3;,吸附过程均为单层吸附且符合Langmuir等温吸附模型和伪二级吸附动力学方程.在溶液浓度40 mg·L-1、甲基橙和亚甲基蓝浓度比3∶1的混合溶液吸附过程中,四方体MgO对甲基橙和亚甲基蓝的去除率分别为80.1;和97.9;.     

纳米CeO2吸附剂的制备及对六价铬的吸附性能

吸附法是去除水中重金属离子的重要方法,开发新型吸附剂一直是研究热点.利用浸渍法和水热法制备了片状和无定形的纳米CeO2吸附剂,探讨其对六价铬的吸附性能,分析pH、吸附时间、六价铬初始浓度等因素对其吸附性能的影响,并通过循环吸附实验考察纳米CeO2吸附剂的再生能力.结果表明:厚度30 nm、直径大小约为400 nm的片状CeO2吸附剂具有更强的吸附能力和更快的吸附速率,80 min时基本达到吸附平衡;两种吸附剂的最佳吸附pH为3;吸附动力学均符合伪二级动力学方程,Langmuir模型和Freundlich模型均能很好地拟合等温吸附过程,表明纳米CeO2对六价铬的吸附以单层吸附为主.片状CeO2四次吸附-解吸实验之后吸附率稍有下降,表明片状CeO2吸附剂有较好的再生能力,因而,该片状CeO2吸附剂适用于与酸性Cr(Ⅵ)废水的处理.     

Identification of the Enzymes Mediating the Maturation of the Seryl-tRNA Synthetase Inhibitor SB-217452 during the Biosynthesis of Albomycins

Albomycin δ₂ is a sulfur-containing sideromycin natural product that shows potent antibacterial activity against clinically important pathogens. The l -serine-thioheptose dipeptide partial structure, known as SB-217452, has been found to be the active seryl-tRNA synthetase inhibitor component of albomycin δ₂. Herein, it is demonstrated that AbmF catalyzes condensation between the 6′-amino-4′-thionucleoside with the d -ribo configuration and seryl-adenylate supplied by the serine adenylation activity of AbmK. Formation of the dipeptide is followed by C3′-epimerization to produce SB-217452 with the d -xylo configuration, which is catalyzed by the radical S-adenosyl-l -methionine enzyme AbmJ. Gene deletion suggests that AbmC is involved in peptide assembly linking SB-217452 with the siderophore moiety. This study establishes how the albomycin biosynthetic machinery generates its antimicrobial component SB-217452.     

Fabrication of Microporous Metal–Organic Frameworks in Uninterrupted Mesoporous Tunnels: Hierarchical Structure for Efficient Trypsin Immobilization and Stabilization

Hierarchically porous metal–organic frameworks (HP-MOFs) are promising in various applications. Most reported HP-MOFs are prepared based on the generation of mesopores in microporous frameworks, and the formed mesopores are connected by microporous channels, limiting the accessibility of mesopores for bulky molecules. A hierarchical structure is formed by constructing microporous MOFs in uninterrupted mesoporous tunnels. Using the confined space in as-prepared mesoporous silica, highly dispersed metal precursors for MOFs are coated on the internal surface of mesoporous tunnels. Ligand vapor-induced crystallization is employed to enable quantitative formation of MOFs in situ, in which sublimated ligands diffuse into mesoporous tunnels and react with metal precursors. The obtained hierarchically porous composites exhibit record-high adsorption capacity for the bulky molecule trypsin. The thermal and storage stability of trypsin is improved upon immobilization on the composites.