Directed Evolution of a Bacterial Laccase (CueO) for Enzymatic Biofuel Cells

Escherichia coli's copper efflux oxidase (CueO) has rarely been employed in the cathodic compartment of enzymatic biofuel cells (EBFCs) due to its low redox potential (0.36 V vs. Ag/AgCl, pH 5.5) towards O₂ reduction. Herein, directed evolution of CueO towards a more positive onset potential was performed in an electrochemical screening system. An improved CueO variant (D439T/L502K) was obtained with a significantly increased onset potential (0.54 V), comparable to that of high‐redox‐potential fungal laccases. Upon coupling with an anodic compartment, the EBFC exhibited an open‐circuit voltage (V_oc) of 0.56 V. Directed enzyme evolution by tailoring enzymes to application conditions in EBFCs has been validated and might, in combination with molecular understanding, enable future breakthroughs in EBFC performance     

Electron–Proton Co‐doping‐Induced Metal–Insulator Transition in VO2 Film via Surface Self‐Assembled l‐Ascorbic Acid Molecules

Charge doping is an effective way to induce the metal–insulator transition (MIT) in correlated materials for many important utilizations, which is however practically limited by problem of low stability. An electron–proton co‐doping mechanism is used to achieve pronounced phase modulation of monoclinic vanadium dioxide (VO₂) at room temperature. Using l ‐ascorbic acid (AA) solution to treat VO₂, the ionized AA^? species donate electrons to the adsorbed VO₂ surface. Charges then electrostatically attract surrounding protons to penetrate, and eventually results in stable hydrogen‐doped metallic VO₂. The variations of electronic structures, especially the electron occupancy of V 3d/O 2p hybrid orbitals, were examined by synchrotron characterizations and first‐principle theoretical simulations. The adsorbed molecules protect hydrogen dopants from escaping out of lattice and thereby stabilize the metallic phase for VO₂.     

Synthesis and Characterization of Some Novel Dendritic Phenothiazine Derivatives

Russian Journal of Organic Chemistry - Three novel dendritic phenothiazine derivatives consisting of a biphenyl core, phenothiazine branching units, and terminal 3,7-di-tert-butylphenothiazine...     

Molecular level comparison of water extractives of maple and oak with negative and positive ion ESI FT‐ICR mass spectrometry

Soluble extractives in wood function to protect living trees from destructive agents and also contribute to wood color and fragrance. Some extractive components have biological activities with medical applications. They also play important roles in wood processing and related applications. To increase the knowledge of wood chemistry, maple and oak were extracted by water. Ultraviolet/visible (UV/vis) spectroscopy indicated the presence of a phenolic compound, resorcinol, in maple extractives having higher molecular mass and more aromatic components than oak extractives. Negative and positive electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry (ESI FT‐ICR‐MS) identified thousands of formulas in the two samples in the m/z range of 200 to 800. They mainly fall into the lignin‐like, carbohydrate‐like, and tannin‐like compound categories. The top 25 peaks (ie, formulas) with the highest relative magnitude in negative ESI represented nearly 50% of the summed total spectral magnitude of all formulas assigned in the maple and oak extractives. Furthermore, the base peak (ie, most abundant peak) accounted for about 14% of the total abundance in each wood sample. Literature comparisons identified 17 of 20 formulas in the top five peaks of the four spectra as specific bioactive compounds in trees and other plants, implying the potential to explore utilization of maple and oak extractives for functional and medicinal applications. The various profiling of the top 25 peaks from the two samples also suggested the possible application of FT‐ICR‐MS for detecting chemical markers useful in profiling and identification of wood types and sources.     

Light-driven circular plasmon current in a silver nanoring

A circular plasmon current in a silver nanoring is demonstrated and investigated with electrodynamics theory. The circular current is driven by the incident plane electromagnetic wave. For a silver ring with a thickness of 50 nm and inner and outer diameters of 200 and 300 nm, the circular current can be obtained when the incident wavelength is at 650 nm, which is about twice the diameter of the ring. The circular current can be observed only when the incident wave and the polarization directions are both parallel to the ring plane. The resonance wavelength shifts to red with the expansion of the ring diameter and the drop in the ring thickness. The discovery holds promise for the design of artificial materials with negative refractive index in the visible wavelengths and might stimulate new ideas for the development of nanoelectronic devices.     

Material point method applied to multiphase flows

The particle-in-cell method (PIC), especially the latest version of it, the material point method (MPM), has shown significant advantage over the pure Lagrangian method or the pure Eulerian method in numerical simulations of problems involving large deformations. It avoids the mesh distortion and tangling issues associated with Lagrangian methods and the advection errors associated with Eulerian methods. Its application to multiphase flows or multi-material deformations, however, encounters a numerical difficulty of satisfying continuity requirement due to the inconsistence of the interpolation schemes used for different phases. It is shown in Section 3 that current methods of enforcing this requirement either leads to erroneous results or can cause significant accumulation of errors. In the present paper, a different numerical method is introduced to ensure that the continuity requirement is satisfied with an error consistent with the discretization error and will not grow beyond that during the time advancement in the calculation. This method is independent of physical models. Its numerical implementation is quite similar to the common method used in Eulerian calculations of multiphase flows. Examples calculated using this method are presented.     

Probing the Contraction and Association of Polystyrene Chains in Semidilute Solution by Non‐Radiative Energy Transfer

The interchain contraction and association of polystyrene in semidilute solution near the Θ temperature are studies using NET. The results reveal that during a drop of temperature, polystyrene chains pass through different states: a smooth change of conformation at temperatures above the Θ temperature, an accelerated contraction and association, aggregation of polymer chains, and then further continuous contraction below the Θ temperature. A pronounced hysteresis is observed during repeated heating. A viscosity study of the same solution was compared with the NET results. It indicates that NET can effectively be used to study conformational changes like contraction and association of polymer chains in a semidilute solution.

     

Isotropic polynomial invariants of Hall tensor

The Hall tensor emerges from the study of the Hall effect, an important magnetic effect observed in electric conductors and semiconductors. The Hall tensor is third-order and three-dimensional, whose first two indices are skew-symmetric. This paper investigates the isotropic polynomial invariants of the Hall tensor by connecting it with a second-order tensor via the third-order Levi-Civita tensor. A minimal isotropic integrity basis with 10 invariants for the Hall tensor is proposed. Furthermore, it is proved that this minimal integrity basis is also an irreducible isotropic function basis of the Hall tensor.     

两端铰接的细长柔性圆柱体涡激振动响应特性数值研究

目前细长柔性圆柱体涡激振动响应的研究方法主要包括实验方法、计算流体动力学方法以及半经验模型方法. 鉴于实验方法研究成本较高、计算流体动力学方法计算时间较长,本文基于尾流振子模型对线性剪切来流下两端铰接的细长柔性圆柱体涡激振动响应特性进行了半经验模型方法研究. 先建立了柔性圆柱体结构振子以及尾流振子之间的耦合模型,紧接着基于二阶精度中心差分格式对耦合模型先离散后迭代进行求解. 对不同剪切参数下柔性圆柱体涡激振动响应的振动波长、振动频率、振动位移以及响应频率随时间的变化特性等参数进行了分析. 分析结果表明:圆柱体的涡激振动响应由驻波和行波混合组成. 当无量纲弯曲刚度较小时,在圆柱体两端附近,驻波占主导;而在圆柱体中间段附近,行波占主导. 当无量纲弯曲刚度较大时,在圆柱体整个长度区间上均为驻波占主导. 随着剪切参数的增大,振动位移以及振动波长均逐渐减小,而振动频率和频率带宽均逐渐增大.