从核心天线到反应中心分子传能研究

利用飞秒时间分辨光谱技术研究了PSⅡ核心复合物内β-Car分子和Chla分子传递光能到反应中心的时间特性.实验测得,在CP47中的β-Car分子用了150 ps,Chla分子用了15 ps;在CP43中β-Car分子用了160 ps,Chla分子用了20 ps.利用超快光谱动力学实验曲线,理论计算出在核心天线中β-Car分子到Chla 662之间的能量传递速率为1.18×10¹²s^-1,β-Car分子到相邻β-Car分子之间按速率 1.14×10¹²s^-1传递能量.理论研究得出,在核心天线中β-Car分子接收到光能,以Dexter电子交换机制和Frster共振传能机制进行激发能传递,最后由Chla分子把能量传递到反应中心,在CP47中用了139 ps,在CP43中用了152 ps.理论研究表明,在核心天线中,Chla分子接收到光能之后,以随机转移方式将能量迅速传递到反应中心P680,在CP47中用了16.8 ps,在CP43中用了18 ps.理论研究与实验研究基本符合.     

A one-step procedure for facile, selective synthesis of protected d-glucopyranosides with free 2-C hydroxyl group starting from peracetylated β-D-glucopyranose

An important field in carbohydrate chemistry is to look for regioselective re-actions of saccharides to simplify the chemical synthesis of oligosaccharides. Oneof such efforts nowadays is directed to the convenient preparation of protected D-     

Facile one-step synthesis of bis(NHC) ruthenium benzylidene catalyst for ring-closing metathesis

Bis(NHC) ruthenium benzylidene complex (H₂IMe)₂(Cl)₂RuCHPh (9) [H₂IMe = 1,3-bis(2,6- dimethylphenyl)-4,5-dihydroimidazol-2-ylidene] was synthesized facilely by one-step reaction of (PPh₃)₂(Cl)₂RuCHPh (7) with N-heterocyclic carbene (NHC) H₂IMe (6). Complex 9 proved to exhibit remarkable catalytic activity for ring-closing metathesis (RCM) reaction at increased temperature.     

Vibrational spectroscopic characterization of 4-acylamidobenzenethiol-stabilized gold nanoparticles

A simple preparation method of gold nanoparticles (AuNPs) with 4-acylamidobenzenethiol derivative (BD) was improved to obtain the larger size of AuNPs which exhibited localized surface plasmon resonance. The spectroscopic characterizations of two kinds of BD-stabilized AuNPs were carried out by means of ATR-FTIR and Raman spectroscopy in order to clarify the conformation and orientation of BDs adsorbed on AuNPs. The relation between the stability of AuNPs and the adsorbed states of BDs were also discussed. The average sizes of the resulting AuNPs were 18 nm for BD1 and 30 nm for BD2, respectively. It was found that the BD1-capped AuNPs formed large aggregates. The results of vibrational spectroscopy revealed that loosely packed self-assembled monolayer (SAM) of BD1 molecules was formed on the surface of the AuNPs; on the other hand, densely packed SAM was formed in the case of BD2. We concluded the difference behavior between the two types of molecules was caused by the functional groups. The sulfuryl groups of BD2 induced highly ordered SAM and suppressed aggregate formation of AuNPs.     

One-step synthesis and applications of fluorescent Cu nanoclusters stabilized by l-cysteine in aqueous solution

Herein, an innovative and simple strategy for synthesizing high fluorescent Cu nanoclusters was successfully established while l-cysteine played a role as the stabilizer. Meaningfully, the current Cu nanoclusters together with a quantum yield of 14.3% were prepared in aqueous solution, indicating their extensive applications. Subsequently, the possible fluorescence mechanism was elucidated by fluorescence, UV–vis, HR-TEM, FTIR, XPS, and MS. Additionally, the CuNCs were employed for assaying Hg²⁺ on the basis of the interactions between Hg²⁺ and l-cysteine; thus facilitating the quenching of their fluorescence. The proposed analytical strategy permitted detections of Hg²⁺ in a linear range of 1.0 × 10⁻⁷ mol L⁻¹ × 10⁻³ mol L⁻¹, with a detection limit of 2.4 × 10⁻⁸ mol L⁻¹ at a signal-to-noise ratio of 3. Significantly, this CuNCs described here were further applied for coding and fluorescent staining, suggesting may broaden avenues toward diverse applications.     

Linear One-Step Processes with Artificial Boundaries

An artificial absorbing boundary is introduced in a linear birth and death stochastic process in order to understand the long time behavior of an ecological community. The solution is obtained by means of a spectral resolution of the probability distribution. A more general linear process with a coefficient of arbitrary strength near the boundary both with absorbing and with reflecting boundary conditions is also studied.     

Properties and biodegradability of water-resistant soy protein/poly(?-caprolactone)/toluene-2,4-diisocyanate composites

Water-resistant composite plastics were prepared from soy protein isolate (SPI) or soy dreg (SD), poly(?-caprolactone) (PCL) and toluene-2,4-diisocyanate (TDI) as the compatibilizer by blending and one-step reactive extrusion (REX) followed by compression-molding. The structure and properties of the materials (SPI series and SD series) were investigated by Fourier transform infrared spectroscopy, scanning electron microscopy, differential scanning calorimetry, dynamic mechanical thermal analysis and tensile testing. The results indicated that SPI and SD series exhibited high water resistance and good tensile strength (14.8 MPa for SPI35 and 16.3 MPa for SD35). Moreover, the SD series sheets containing cellulose possessed higher tensile strength than those of SPI series when SD content was 30-35%, whereas the latter had a better biodegradability and water resistance. By burying the two series of sheets in soil and culturing them in a mineral salt medium containing microorganisms, both of them were almost completely degraded. This paper provides a convenient way to prepare new soy protein plastics with good biodegradability and water resistivity.     

Comparative studies on zirconia and graphene composites obtained by one-step and stepwise electrodeposition for deoxyribonucleic acid sensing

In this paper, the comparison of two kinds of electrochemically reduced graphene oxide (ERGNO) and zirconia composites, obtained by one-step (ZrO₂–ERGNO) and stepwise (ZrO₂/ERGNO) electrodeposition for DNA sensing, is systematically studied. The resulting composites were characterized by scanning electron microscopy, cyclic voltammetry, and differential pulse voltammetry. The results indicated that the ZrO₂–ERGNO presented fine globular nanostructure. However, ZrO₂/ERGNO presented agglomerate massive microstructure due to the absence of the oxygen-containing groups of graphene oxide, confirming the oxygen-containing groups provided a better affinity for the deposition of ZrO₂. Due to the strong binding of the phosphate groups of DNA with the zirconia film, DNA probes were attached on the ZrO₂-based composites. ZrO₂–ERGNO/Au owning fine nanostructure presented larger surface area than microstructured ZrO₂/ERGNO/Au. Moreover, compared with microstructured ZrO₂/ERGNO, the nanostructured ZrO₂–ERGNO provided more accessible space for immobilized DNA probe hybridization with target sequence, which consequently resulted in higher hybridization efficiency. Therefore, the ZrO₂–ERGNO was chosen for fabricating DNA sensor with a limit of detection 1.21 × 10⁻¹⁴ mol L⁻¹.     

A one-step method for producing microencapsulated phase change materials

This short communication reports our recent work on the synthesis and characterisation ofmicrocapsules of phase change materials using silica as the shell material through a one-step method. The method uses no surfactants or dispersants for stabilising the capsules. The results show that the one-step method allows the tuning of the size and polydispersity of the capsules, and the use of different core materials. Analyses of the capsules show that they contain about 65% phase change materials. The results also suggest no need for a stabilising agent due to self-stabilisation by the amine groups. Further work is underway to investigate the mechanical and thermal properties of the microcapsules and the scale-up of the method.     

One-step synthesis of novel biacidic carbon via hydrothermal carbonization

The novel biacidic carbon has been synthesized via one-step hydrothermal carbonization of glucose, citric acid, and hydroxyethylsulfonic acid at 180 °C for only 4 h. The novel carbon had an acidity of 1.7 mmol/g with the carbonyl to sulfonic acid groups molar ratio of 1:3, which was confirmed by IR, XPS, TPD, SEM, and BET analyses. The catalytic activities of the carbon were investigated through esterification and oxathioketalization. The results showed that the carbon owned the comparable activities to sulfuric acid, which indicated that the carbon holds great potential for the green processes.