Directed Molecular Collection by E‐Jet Printed Microscale Chemical Potential Wells in Hydrogel Films

A facile approach to locally concentrate analytes of interest will significantly enhance miniaturized, integrated chemical‐analysis systems. Here, the directed analyte transport and concentration using ≈200 µm‐diameter E‐jet printed chemical potential wells in a polyacrylamide hydrogel is demonstrated. Using a cationic well as the model system, anionic analytes are accumulated into a microscale area with a local concentration enhancement of >50‐fold relative to the surrounding area. By downscaling the diameter of the chemical potential well from a few millimeters to 100s of micrometers, it is found, using both fluorescence and Raman microscopy, that the molecular collection capacity of the well is greatly improved. Additionally, it is shown that molecules can be simultaneously transported and concentrated to arrays of microscale regions using an array of microscale chemical potential wells. This approach enhances many‐fold the limit of detection, enables the formation of microscale potential well arrays with a variety of chemical properties, and provides a novel microscale molecular manipulation technique as an alternative to traditional microfluidic‐based systems.     

改性淀粉抑制赤铁矿反浮选石英的作用机理研究

通过矿物浮选试验、动电位测定以及吸附量测试,考察了4种淀粉抑制剂对赤铁矿和石英浮选性能的影响,并探讨了其作用机理。在碱性条件下,改性淀粉抑制剂对赤铁矿抑制效果明显,且以改性玉米淀粉效果最佳,改性磷酸酯淀粉、改性羧甲基淀粉的抑制效果次之,而普通淀粉抑制作用一般。同时4种淀粉抑制剂对主要脉石矿物石英的抑制效果均不明显。pH=10~12.5条件下,改性玉米淀粉因其羟基氧和裸露在赤铁矿表面的铁元素发生了化学键合,因而选择性抑制能力最佳。分子动力学模拟表明,改性玉米淀粉片段与赤铁矿作用更为紧密,验证了改性淀粉能更好地抑制赤铁矿。     

Modeling Alcohol Dehydrogenase Catalysis in Deep Eutectic Solvent/Water Mixtures

The use of oxidoreductases (EC1) in non-conventional reaction media has been increasingly explored. In particular, deep eutectic solvents (DESs) have emerged as a novel class of solvents. Herein, an in-depth study of bioreduction with an alcohol dehydrogenase (ADH) in the DES glyceline is presented. The activity and stability of ADH in mixtures of glyceline/water with varying water contents were measured. Furthermore, the thermodynamic water activity and viscosity of mixtures of glyceline/water have been determined. For a better understanding of the observations, molecular dynamics simulations were performed to quantify the molecular flexibility, hydration layer, and intraprotein hydrogen bonds of ADH. The behavior of the enzyme in DESs follows the classic dependence of water activity (a_W) in non-conventional media. At low a_W values (<0.2), ADH does not show any activity; at higher a_W values, the activity was still lower than that in pure water due to the high viscosities of the DES. These findings could be further explained by increased enzyme flexibility with increasing water content.     

Sequence-Dependent Nanofiber Structures of Phenylalanine and Isoleucine Tripeptides

The molecular design of short peptides to achieve a tailor-made functional architecture has attracted attention during the past decade but remains challenging as a result of insufficient understanding of the relationship between peptide sequence and assembled supramolecular structures. We report a hybrid-resolution model to computationally explore the sequence–structure relationship of self-assembly for tripeptides containing only phenylalanine and isoleucine. We found that all these tripeptides have a tendency to assemble into nanofibers composed of laterally associated filaments. Molecular arrangements within the assemblies are diverse and vary depending on the sequences. This structural diversity originates from (1) distinct conformations of peptide building blocks that lead to different surface geometries of the filaments and (2) unique sidechain arrangements at the filament interfaces for each sequence. Many conformations are available for tripeptides in solution, but only an extended β-strand and another resembling a right-handed turn are observed in assemblies. It was found that the sequence dependence of these conformations and the packing of resulting filaments are determined by multiple competing noncovalent forces, with hydrophobic interactions involving Phe being particularly important. The sequence pattern for each type of assembly conformation and packing has been identified. These results highlight the importance of the interplay between conformation, molecular packing, and sequences for determining detailed nanostructures of peptides and provide a detailed insight to support a more precise design of peptide-based nanomaterials.     

介孔分子硅剂改善茶浓缩膜结构特性应用研究

为有效提高功能性茶浓缩反渗透膜的回收效率和抗污性能,探究了3种介孔分子硅材料(MCM-41、SBA-15和MCFs)对浓缩膜面聚酰胺层聚合形成过程的结构影响。结果表明,添加质量分数0.02%经磺化预处理的MCM-41于间苯二胺水相可接枝酰氯基团,形成的聚酰胺结构层峰谷粗糙跨度仅为220 nm且交联紧致,膜抗拉伸强度增加37.8%;SBA-15和MCFs相膜面峰谷跨度达500~780 nm,横向褶皱和团聚,结构存在孔道塌陷;改性膜在3 h内对茶多酚、茶多糖、茶蛋白即可达到最大浓缩度,减少50%浓缩时间;MCM-41和SBA-15膜长时间运行的浓缩降率仅为2.8%~6.1%,48 h下降率比显示改性膜达标使用时长增加112.5%~137.5%,亲水性和抗污堵能力均大幅提升,可有效满足功能化茶浓缩精度。     

Activity-Directed Synthesis: A Flexible Approach for Lead Generation

Activity-directed synthesis (ADS) is a structure-blind, functional-driven molecular discovery approach. In this Concept, four case studies highlight the general applicability of ADS and showcase its flexibility to support different medicinal chemistry strategies. ADS deliberately harnesses reactions with multiple possible outcomes, and allows many chemotypes to be evaluated in parallel. Resources are focused on bioactive molecules, which emerge in tandem with associated synthetic routes. Some of the future challenges for ADS are highlighted, including the realisation of an autonomous molecular discovery platform. The prospects for ADS to become a mainstream lead generation approach are discussed.     

Safe preparation of beefy meaty peptide with Bacillus subtilis

Preparation of flavour peptides with microorganisms is an attractive choice for its large-scale production. However, beefy meaty peptide (BMP), as a research hotspot in the field of umami peptide, has been studied in few microorganisms, and furthermore, the safe preparation of BMP has not yet been reported. In this study, multi-copy BMP (8BMP) was successfully expressed and produced in the ‘generally recognized as safe’ Bacillus subtilis (B. subtilis). Firstly, 8BMP with the potentially intense umami was screened out based on molecular docking analysis. Then, it was successfully expressed in the B. subtilis 168 and verified through sensory evaluation. Finally, the scaling capacity of 8BMP was evaluated in a 5-L fermenter, with the highest yield (0.84 g L⁻¹) 6.4 times than that of shake flask, which is conductive for industrial production of BMP and other food peptides.