New lead-iodide formates with a strong second-harmonic generation response and suitable birefringence obtained by the substitution strategy

Nonlinear optical (NLO) crystals featuring a strong second-harmonic generation (SHG) response and suitable birefringence to achieve phase-matching are in urgent demand in industrial and commercial applications. Based on the substitution strategy, two new NLO lead-iodide formates, K₂[PbI₂(HCOO)₂] and Rb₂[PbI₂(HCOO)₂], have been successfully synthesized using a moderate mixed-solvothermal method. K₂[PbI₂(HCOO)₂] and Rb₂[PbI₂(HCOO)₂] exhibit strong phase-matching SHG responses of 8 and 6.8 × KDP, respectively, a suitable birefringence and transparent window covering most of the visible light and mid-IR region. Crystal structures and theoretical calculations unveil that the origins of the strong SHG response and suitable birefringence can be credibly attributed to the oriented arrangement of the highly distorted [PbI₂O₄] hexa-coordinated polyhedra, which are consistent in their local dipole moments, as well. This research provides a new strategy to explore high-performance NLO crystals.

K₂[PbI₂(HCOO)₂] and Rb₂[PbI₂(HCOO)₂] with highly distorted [PbI₂O₄] polyhedra in an oriented arrangement exhibit a very strong phase-matching SHG response, suitable birefringence, wide transparent windows and good thermal stability.     

A vending machine for drug-like molecules – automated synthesis of virtual screening hits

As a result of high false positive rates in virtual screening campaigns, prospective hits must be synthesised for validation. When done manually, this is a time consuming and laborious process. Large “on-demand” virtual libraries (>7 × 10¹² members), suitable for preparation using capsule-based automated synthesis and commercial building blocks, were evaluated to determine their structural novelty. One sub-library, constructed from iSnAP capsules, aldehydes and amines, contains unique scaffolds with drug-like physicochemical properties. Virtual screening hits from this iSnAP library were prepared in an automated fashion for evaluation against Aedes aegypti and Phytophthora infestans. In comparison to manual workflows, this approach provided a 10-fold improvement in user efficiency. A streamlined method of relative stereochemical assignment was also devised to augment the rapid synthesis. User efficiency was further improved to 100-fold by downscaling and parallelising capsule-based chemistry on 96-well plates equipped with filter bases. This work demonstrates that automated synthesis consoles can enable the rapid and reliable preparation of attractive virtual screening hits from large virtual libraries.

A compact and operationally simple automation technology can prepare virtual screening hits from a large on-demand library of drug-like molecules.     

哈密顿系统正则变换在时变最优控制中的应用

利用哈密顿系统正则变换和生成函数理论求解线性时变最优控制问题,构造了新的最优控制律形式并提出了控制增益计算的保结构算法. 利用生成函数求解最优控制导出的哈密顿系统两端边值问题,并构造线性时变系统的最优控制律,由第2类生成函数所构造的最优控制律避免了末端时刻出现无穷大反馈增益. 控制系统设计中需求解生成函数满足的时变矩阵微分方程组. 根据生成函数与哈密顿系统状态转移矩阵之间的关系,从正则变换的辛矩阵描述出发,导出了求解这组微分方程组的保结构递推算法.为了保持递推计算中的辛矩阵结构,哈密顿系统状态转移矩阵的计算中利用了Magnus级数.      

A new method for solving Biot＇s consolidation of a finite soil layer in the cylindrical coordinate system

A new method is developed to solve Biot＇s consolidation of a finite soil layer in the cylindrical coordinate system. Based on the governing equations of Biot＇s consolidation and the technique of Laplace transform, Fourier expansions and Hankel transform with respect to time t, coordinate θ and coordinate r, respectively, a relationship of displacements, stresses, excess pore water pressure and flux is established between the ground surface （z = 0） and an arbitrary depth z in the Laplace and Hankel transform domain. By referring to proper boundary conditions of the finite soil layer, the solutions for displacements, stresses, excess pore water pressure and flux of any point in the transform domain can be obtained. The actual solutions in the physical domain can be acquired by inverting the Laplace and the Hankel transforms.     

Minimum-time optimal control of robotic manipulators based on Hamel’s integrators

Meccanica - In this paper, we develop a framework of time optimization path planning for robotic manipulators surrounded by static obstacles. Our approach is based on the recursive dynamics method...     

Switched-model-based compound control of hypersonic vehicles with input nonlinearities

Nonlinear Dynamics - Focusing on the large-envelope control problem of air-breathing hypersonic vehicles (AHVs), this paper employs a switched control-oriented model (SCOM) to describe vehicle...     

Highly effective and chemoselective hydrodeoxygenation of aromatic alcohols

Effective hydrodeoxygenation (HDO) of aromatic alcohols is very attractive in both conventional organic synthesis and upgrading of biomass-derived molecules, but the selectivity of this reaction is usually low because of the competitive hydrogenation of the unsaturated aromatic ring and the hydroxyl group. The high activity of noble metal-based catalysts often leads to undesired side reactions (e.g., saturation of the aromatic ring) and excessive hydrogen consumption. Non-noble metal-based catalysts suffer from unsatisfied activity and selectivity and often require harsh reaction conditions. Herein, for the first time, we report chemoselective HDO of various aromatic alcohols with excellent selectivity, using porous carbon–nitrogen hybrid material-supported Co catalysts. The C–OH bonds were selectively cleaved while leaving the aromatic moiety intact, and in most cases the yields of targeted compounds reached above 99% and the catalyst could be readily recycled. Nitrogen doping on the carbon skeleton of the catalyst support (C–N matrix) significantly improved the yield of the targeted product. The presence of large pores and a high surface area also improved the catalyst efficiency. This work opens the way for efficient and selective HDO reactions of aromatic alcohols using non-noble metal catalysts.

Porous carbon–nitrogen hybrid material-supported Co catalysts can effectively promote the chemoselective hydrodeoxygenation reaction of a various of aromatic alcohols in ethanol and hydrogen atmosphere, under relatively mild conditions.