甘油氧化的光谱电化学傅里叶变换衰减全反射谱红外光谱薄膜流动池中硼酸镍层厚度的优化

在碱性甘油电氧化反应中,利用电化学傅里叶变换衰减全反射谱红外光谱法,研究了薄膜流动池中滴注硼酸镍催化剂负载量对玻碳电极性能的影响.连续操作的径向流动池包括一个位于内反射元件上方50μm的钻孔电极,可实现红外光谱分析.这是在确定条件下对电催化剂进行简便和可重复筛选的一个适合的方法,同时还提供了对复杂反应(如甘油氧化)产物选择性的检测.通过对泵送电解液进行更耗时的定量高效液相色谱分析,结果表明,衰减全反射红外光谱法可快速鉴定产物.在层流条件下,水中使用0.1 M甘油和1 M KOH,流速为5μL min-1时,甘油转化率较高.转化率和选择性取决于催化剂的负载量,负载量又决定了催化剂层的厚度和粗糙度.由于在更粗糙的膜中停留时间更长有利于再吸附和C-C键断裂,因此当负载量最高达210μg cm-2时,甘油转化率为73％且甲酸选择性接近80％.当最低负载量为13μg cm-2时,甘油转化率达到63％,甲酸选择性降至60％,相应地,C2物种(如乙醇酸盐)选择性较高,为8％.因此,只有催化剂负载量较低时才能形成几微米厚度范围内的薄膜,此时才适合进行优质催化剂的筛选.     

Identification of predominant point defects in nonstoichiometric CuInse2 by X-ray powder diffraction

Refinement of structural parameter, occupancy factors and temperature factors of three indium rich samples enabled type and concentration of intrinsic point defects to be determined. Vacancies on copper and indium sites (8 and 5%, respectively) and indium atoms on copper sites (5%) were identified. Indium atoms exhibit a large thermal vibration amplitude.     

Bulk flow in ferrofluids in a uniform rotating magnetic field

Direct measurements of the bulk flow of a ferrofluid in a uniform rotating magnetic field were obtained using the ultrasonic velocity profile method. The fluid was observed to corotate with the field in a rigid-body-like fashion throughout the bulk of the container, except near the air-fluid interface, where it was observed to counterrotate. The results were found in qualitative agreement with the spin diffusion theory of Zaitsev and Shliomis [J. Appl. Mech. Tech. Phys. 10, 696 (1969)]10.1007/BF00907424.     

Using light to bioactivate surfaces: A new way of creating oriented, active immunobiosensors

Ultraviolet light can be used to immobilize biomolecules onto thiol reactive surfaces in order to, e.g., make biosensors. The mechanism involves light-induced formation of free, reactive thiol groups in disulphide containing molecules. This technology allows for the creation of arrays of biomolecules with a high degree of reproducibility, circumventing the need for often expensive nano/micro-dispensing technologies. The ultimate size of the immobilized spots is defined by the focal area of the UV beam. Light-induced immobilization has the added benefit that the immobilized molecules will be spatially oriented and covalently bound to the surface. In this paper, we demonstrate the utility of a sensor array created with the new sensor technology when integrated into a microfluidic system. Protein arrays made using light-induced immobilization showed successful antigen/antibody binding in a flow cell allowing the visualisation of real time binding and enzyme activity. This new technology is ideal for the creation of protein/DNA microarrays, can replace present micro-dispensing arraying technologies and is ideal as a molecular imprinting technology.     

Experimental realization of an order-finding algorithm with an NMR quantum computer

We report the realization of a nuclear magnetic resonance quantum computer which combines the quantum Fourier transform with exponentiated permutations, demonstrating a quantum algorithm for order finding. This algorithm has the same structure as Shor's algorithm and its speed-up over classical algorithms scales exponentially. The implementation uses a particularly well-suited five quantum bit molecule and was made possible by a new state initialization procedure and several quantum control techniques.     

Raman scattering of Ge dot superlattices

Self-organised Ge dot superlattices grown by molecular beam epitaxy of Ge and Si layers utilizing Stranski-Krastanov growth mode were investigated by Raman spectroscopy. An average size of Ge quantum dots was obtained from transmission electron microscopy measurements. The strain and interdiffusion of Ge and Si atoms in Ge quantum dots were estimated from the analysis of frequency positions of optical phonons observed in the Raman spectra. Raman scattering by folded longitudinal acoustic phonons in the Ge dot superlattices was observed and explained using of elastic continuum theory. Received 25 January 2000     

Resonant Raman scattering by strained and relaxed germanium quantum dots

This paper reports on the results of resonant Raman scattering investigations of the fundamental vibrations in Ge/Si structures with strained and relaxed germanium quantum dots. Self-assembled strained Ge/Si quantum dots are grown by molecular-beam epitaxy on Si(001) substrates. An ultrathin SiO₂ layer is grown prior to the deposition of a germanium layer with the aim of forming relaxed germanium quantum dots. The use of resonant Raman scattering (selective with respect to quantum dot size) made it possible to assign unambiguously the line observed in the vicinity of 300 cm^?1 to optical phonons confined in relaxed germanium quantum dots. The influence of confinement effects and mechanical stresses on the vibrational spectra of the structures with germanium quantum dots is analyzed.     

Bridging the Green Gap: Metal–Organic Framework Heteromultilayers Assembled from Porphyrinic Linkers Identified by Using Computational Screening

In organic photovoltaics, porphyrins (PPs) are among the most promising compounds owing to their large absorption cross-section, wide spectral range, and stability. Nevertheless, a precise adjustment of absorption band positions to reach a full coverage of the so-called green gap has not been achieved yet. We demonstrate that a tuning of the PP Q- and Soret bands can be carried out by using a computational approach for which substitution patterns are optimized in silico. The most promising candidate structures were then synthesized. The experimental UV/Vis data for the solvated compounds were in excellent agreement with the theoretical predictions. By attaching further functionalities, which allow the use of PP chromophores as linkers for the assembly of metal-organic frameworks (MOFs), we were able to exploit packing effects resulting in pronounced redshifts, which allowed further optimization of the photophysical properties of PP assemblies. Finally, we use a layer-by-layer method to assemble the PP linkers into surface-mounted MOFs (SURMOFs), thus obtaining high optical quality, homogeneous and crystalline multilayer films. Experimental results are in full accord with the calculations, demonstrating the huge potential of computational screening methods in tailoring MOF and SURMOF photophysical properties.