Mass spectrometry imaging for biomedical applications

The development of technologies for mass spectrometry imaging is of substantial research interest. Mass spectrometry is potentially capable of providing highly specific information about the distribution of compounds in tissues, with high sensitivity. The in-situ analysis needed for tissue imaging requires MS to be performed under conditions different from the traditional ones, typically with intensive sample preparation and optimized for pharmaceutical applications. In this paper we critically review the current status of MS imaging with different methods of sample ionization and discuss the 3D and quantitative imaging capabilities which need further development, the importance of the multi-modal imaging, and the balance between the pursuit of high-resolution imaging and the practical application of MS imaging in biomedicine.     

Electrochemical separation of uranium and cerium in molten LiCl–KCl

The electrochemical separation of uranium from cerium in LiCl–KCl eutectic and the electrochemical behavior of Ce(III) were studied. According to the cyclic voltammogram of Ce(III) and the former result of U(III), electrodeposition potential was determined at ?1.65 V (vs Ag/AgCl). The uranium metal was successfully deposited and separated from cerium. The morphology of deposit and cross section of electrode were investigated by SEM, firstly uranium deposit alloys with stainless steel and forms a thin transition layer, and secondly the uranium metal layer grows from the transition layer. The separation factors of uranium/cerium on different recovery ratios were determined through a series of steps. It was found that the content of cerium in the deposit and separation factors declined with increasing the initial concentration of U³⁺ in molten salts; the separation factors remained stable at around 20 in different uranium recovery ratios.     

Quantitative Investigation on Structural Evolution of Co-continuous Phase under Shear Flow

Components of co-continuous phase can form an interpenetrating network structure, which has great potential to synergistically improve the mechanical properties of the blends, and to impart the functional blends superior electrical conductivity and permeability. In this work, the effects of shear rates (50–5000 s^?1) at different temperatures on the phase morphology, phase size and lamellar crystallites of biodegradable co-continuous polybutylene terephthalate (PBAT)/polybutylene succinate (PBS) blend are quantitatively investigated. The results show that the above features of the PBAT/PBS have a strong dependence on the shear flow and thermal field. The co-continuous phase of the blend is well maintained at 130 °C. Interestingly, this phase structure transforms into a “sea-island” structure at 160 °C, which gradually recovers to a co-continuous phase when the shear rate increases from 1000 s^?1 to 5000 s^?1. The phase size decreases with the increase of shear rate both at 130 °C and 160 °C due to the refinement and deformation of phase structures caused by strong shear stress. Unexpectedly, a unique phenomenon is observed that the shear-induced lamellar crystallites are oriented perpendicular to shear direction in the range of 500–5000 s^?1 at 130 °C, while the orientation of lamellar crystallites at 160 °C is along the shear direction within the whole range of shear rates. The degree of orientation for the PBAT/PBS blend crystals increases first and then decreases at both temperatures above. In addition, the range of shear rate has reached the level in the industrial processing. Therefore, this work has important guiding significance for the regulation of the co-continuous phase structure and the performance for the blend in the practical processing.

     

Quantitative analysis of asymmetrical cortical activity in motor areas during sequential finger movement

Brain asymmetry is a phenomenon well known for handedness and has been studied in motor cortices. However, few quantitative studies on asymmetrical cortical activity in motor areas have been conducted. In this study, we systematically investigated asymmetrical cortical activity in motor areas during sequential finger movement by quantitatively analyzing functional magnetic resonance imaging (fMRI) blood oxygenation level-dependent (BOLD) responses. The norm of BOLD signal percentage of change was introduced to quantitatively measure the BOLD signal intensity change difference between the left and right motor areas. The results of the data collected from six subjects show that the norm of BOLD signal percentage of change in the right motor area is higher than that in the left motor area for two-hand movement (P=.0059) and single-hand movement (P=.0279) with right-handedness. These results from fMRI show the asymmetry of motor areas and may suggest that the left hemisphere motor area comes into being as an adaptation system that needs few neuron cells only to finish any movement task for right-handedness. The activation intensity in the left motor area is reduced with normal right finger movement. The activation intensity in the right motor area is obviously higher than that in the left motor area.     

DNA Nanoribbon-Templated Self-Assembly of Ultrasmall Fluorescent Copper Nanoclusters with Enhanced Luminescence

Fluorescent copper nanoclusters (CuNCs) have been widely used in chemical sensors, biological imaging, and light-emitting devices. However, individual fluorescent CuNCs have limitations in their capabilities arising from poor photostability and weak emission intensities. As one kind of aggregation-induced emission luminogen (AIEgen), the formation of aggregates with high compactness and good order can efficiently improve the emission intensity, stability, and tunability of CuNCs. Here, DNA nanoribbons, containing multiple specific binding sites, serve as a template for in situ synthesis and assembly of ultrasmall CuNCs (0.6 nm). These CuNC self-assemblies exhibit enhanced luminescence and excellent fluorescence stability because of tight and ordered arrangement through DNA nanoribbons templating. Furthermore, the stable and bright CuNC assemblies are demonstrated in the high-sensitivity detection and intracellular fluorescence imaging of biothiols.     

Water-Soluble Polymers with Appending Porphyrins as Bioinspired Catalysts for the Hydrogen Evolution Reaction

Molecular design to improve catalyst performance is significant but challenging. In enzymes, residue groups that are close to reaction centers play critical roles in regulating activities. Using this bioinspired strategy, three water-soluble polymers were designed with appending Co porphyrins and different side-chain groups to mimic enzyme reaction centers and activity-controlling residue groups, respectively. With these polymers, high hydrogen evolution efficiency was achieved in neutral aqueous media for electro- (turnover frequency >2.3×10⁴ s⁻¹) and photocatalysis (turnover number >2.7×10⁴). Porphyrin units are surrounded and protected by polymer chains, and more importantly, the activity can be tuned with different side-chain groups. Therefore, instead of revising molecular structures that is difficult from both design and synthesis points of view, polymers can be used to improve molecular solubility and stability and simultaneously regulate activity by using side-chain groups.     

手性环丙烯构建策略用于对映选择性合成偕二氟亚甲基三元环化合物

作为最小的不饱和环状分子,环丙烯独特的刚性结构和多变的反应活性吸引了化学家的研究兴趣.自1922年Demjanov[1]报道了环丙烯化合物的首例合成以来,现已发展了一系列环丙烯的合成方法.手性环丙烯的合成是通过炔烃和重氮化合物的[2+1]不对称环加成反应.根据底物的不同,这些不对称环加成反应可以分为四类:(a)末端炔烃和单取代重氮化合物的反应,(b)末端炔烃和双取代重氮化合物的反应,(c)非末端炔烃和双取代重氮化合物的反应,(d)非末端炔烃和单取代重氮化合物的反应.在这四类反应中,末端炔烃和单取代重氮化合物的不对称反应相对容易进行.1992年,Doyle和Müller等[2]报道了手性铑催化剂[Rh2(5R-MEPY)4]促进的末端炔烃和重氮醋酸酯之间的不对称环丙烯基化反应(Scheme 1a).随后各种手性催化剂包括[Rh2(OAc)-(DPTI)3][3]、Ir(salen)衍生物[4]和[Co(3,5-diMes-Chen-Phyrin)][5]等被先后报道用于末端炔烃和单取代重氮化合物的不对称[2+1]环加成反应.     

Behaviour of silicon ointment for power-cable insulation under external heating

Journal of Thermal Analysis and Calorimetry - The burning process and typical fire parameters of power-cable silicon ointment were explored experimentally using a cone calorimeter, and the effects...     

Comparison of the active components of Aster tataricus from different regions and related processed products by ultra‐high performance liquid chromatography with tandem mass spectrometry

We investigated crude Aster tataricus, vinegar‐processed Aster tataricus, honey‐processed Aster tataricus, and steamed Aster tataricus as a case study and developed a comprehensive strategy integrating quantitative analysis and chemical pattern recognition methods for the evaluation and differentiation of Aster tataricus from different regions, as well as related processed products. In the study, 15 batches of raw Aster tataricus collected from seven provinces were analyzed. A sensitive and rapid ultra‐high performance liquid chromatography with tandem mass spectrometry method for simultaneous determination of 15 compounds was established to evaluate the quality of raw and processed Aster tataricus. Furthermore, multivariate statistical techniques were applied to compare the differences among Aster tataricus samples. As a result, the herbs collected from seven provinces were divided into two categories, and chlorogenic acid was the most important component distinguishing between the regions. Moreover, all of the raw and processed samples were classified by partial least squares discriminant analysis based on the 15 analyzed compounds. Results showed that raw Aster tataricus, vinegar‐processed Aster tataricus, honey‐processed Aster tataricus, and steamed Aster tataricus were clustered in four different areas. Shionone, chlorogenic acid and kaempferol were the significant constituents differentiating the raw and differently processed Aster tataricus samples.