Na2S-Mediated One-Pot Selective Deoxygenation of α-Hydroxyl Carbonyl Compounds including Natural Products

A practical method for the deoxygenation of α-hydroxyl carbonyl compounds under mild reaction conditions is reported here. The use of cheap and easy-to-handle Na₂S·9H₂O as the reductant in the presence of PPh₃ and N-chlorosuccinimide (NCS) enables the selective dehydroxylation of α-hydroxyl carbonyl compounds, including ketones, esters, amides, imides and nitrile groups. The synthetic utility is demonstrated by the late-stage deoxygenation of bioactive molecule and complex natural products.     

Pattern-adaptive error diffusion algorithm for improved phase-only hologram generation

The bidirectional error diffusion(BERD) algorithm is free from random phase modulation that introduces speckle noise on the reconstructed images, compared with other computer-generated phase-only hologram(POH) approaches. During the POH generation process, the amplitudes of all pixels are traditionally set to one for diffusing the errors to their neighborhood of unprocessed pixels. In this paper, we reveal that the reconstruction quality depends on the uniform amplitude value for different object pattern. The pattern-adaptive BERD(PA-BERD) algorithm is proposed for high-quality holographic reconstruction. The optimized amplitude value can be acquired for each object pattern and each propagation distance.The PA-BERD-based POHs have shown higher reconstruction quality than traditional BERD-based POHs in simulations as well as optical experiments.     

Unraveling hydridic-to-protonic dihydrogen bond predominance in monohydrated dodecaborate clusters

Hydridic-to-protonic dihydrogen bonds (DHBs) are involved in comprehensive structural and energetic evolution, and significantly affect reactivity and selectivity in solution and solid states. Grand challenges exist in understanding DHBs’ bonding nature and strength, and how to harness DHBs. Herein we launched a combined photoelectron spectroscopy and multiscale theoretical investigation using monohydrated closo-dodecaborate clusters B₁₂X₁₂²⁻·H₂O (X = H, F, I) to address such challenges. For the first time, a consistent and unambiguous picture is unraveled demonstrating that B–H⋯H–O DHBs are superior to the conventional B–X⋯H–O HBs, being 1.15 and 4.61 kcal mol⁻¹ stronger than those with X = F and I, respectively. Energy decomposition analyses reveal that induction and dispersion terms make pronounced contributions resulting in a stronger B–H⋯H–O DHB. These findings call out more attention to the prominent roles of DHBs in water environments and pave the way for efficient and eco-friendly catalytic dihydrogen production based on optimized hydridic-to-protonic interactions.

A joint gas-phase ion spectroscopic and multiscale theoretical study reveals unequivocally the predominance of the hydridic-to-protonic dihydrogen bond over the prototypical strong hydrogen bond in monohydrated dodecaborate clusters.     

导电性磁流变弹性体的研究进展

磁流变弹性体(magnetorheological elastomer,MRE)因其独特的场相关性能在工程应用领域引起了广泛关注.论文介绍了MRE的最新发展,重点介绍导电性MRE在材料设计、力学行为和实际应用等方面的研究现状.论文从高性能导电性MRE的研制开始,讨论了材料与结构设计中涉及的关键问题;介绍了导电性MRE材料在磁场作用下的磁、力、电学行为的耦合作用机理和相关物理模型;之后对导电性MRE器件的研究现状进行了总结;最后展望了导电性MRE的发展潜力和面临的挑战.     

轴承自供能监测的径向电磁式能量俘获建模与实验研究

无线网络和低功耗微电子技术的进步推动着设备健康监测技术的网联化和智能化发展.轴承作为旋转设备的关键部件,对国防、轨道交通、风电等重大装备的健康状态起到了非常重要的作用,实现轴承状态监测的微型化和自供能是装备智能化的重要技术基础.论文针对于轴承无线传感器网络的供能问题,提出了一种用于轴承自供能监测的径向电磁式旋转能量俘获建模方法,并通过引入环形Halbach永磁阵列增强了线圈中的磁场强度,提高了能量俘获系统的输出性能.基于磁荷理论和空间坐标变换给出了环形Halbach永磁阵列的径向磁场计算方法,进而利用电磁感应原理建立了电磁式旋转能量俘获系统的输出电压模型,仿真分析了不同参数对系统输出电压的影响.有限元仿真和不同转速下的实验结果验证了所建立模型预测输出电压的准确性,同时功率测试实验表明设计的俘能系统在1000 rpm转速下可实现81.2 mW的输出功率.     

神光Ⅱ装置上辐射驱动瑞利-泰勒不稳定性实验

在神光Ⅱ装置上开展了辐射驱动RT不稳定性的一系列实验,获得了不同初始扰动幅度、不同扰动波长、不同材料样品等条件下辐射烧蚀RT不稳定性增长的高时空分辨背光图像,特别是在大初始扰动幅度样品实验中获得了扰动增长的清晰图像,观察到了扰动增长从线性区到非线性区的过渡过程,二次和三次谐波的产生和发展清楚可见。充实了数值模拟程序考核的实验数据库,对间接驱动ICF点火靶设计和研究具有重要作用。     

A Novel Aptamer-Imprinted Polymer-Based Electrochemical Biosensor for the Detection of Lead in Aquatic Products

Lead contamination in aquatic products is one of the main hazard factors. The aptasensor is a promising detection method for lead ion (Pb(II)) because of its selectivity, but it is easily affected by pH. The combination of ion-imprinted polymers(IIP) with aptamers may improve their stability in different pH conditions. This paper developed a novel electrochemical biosensor for Pb(II) detection by using aptamer-imprinted polymer as a recognition element. The glassy carbon electrode was modified with gold nanoparticles and aptamers. After the aptamer was induced by Pb(II) to form a G-quadruplex conformation, a chitosan-graphene oxide was electrodeposited and cross-linked with glutaraldehyde to form an imprint layer, improving the stability of the biosensor. Under the optimal experimental conditions, the current signal change (∆I) showed a linear correlation of the content of Pb(II) in the range of 0.1–2.0 μg/mL with a detection limit of 0.0796 μg/mL (S/N = 3). The biosensor also exhibited high selectivity for the determination of Pb(II) in the presence of other interfering metal ion. At the same time, the stability of the imprinted layer made the sensor applicable to the detection environment with a pH of 6.4–8.0. Moreover, the sensor was successfully applied to the detection of Pb(II) in mantis shrimp.     

Natural Antioxidants,Tyrosinase and Acetylcholinesterase Inhibitors from Cercis glabra Leaves

Cercis glabra is a plant belonging to the legume family, whose flowers and barks are commonly used as food and traditional Chinese medicines. However, its leaves are usually disposed of as wastes. This research comprehensively investigated the bioactive constituents of C. glabra leaves, and two new phenolic, ceroffesters A-B (1–2) and thirteen known compounds (3–15) were isolated. Their structures were elucidated by spectroscopic methods such as nuclear magnetic resonance (1D NMR and 2D NMR), high-resolution electrospray ionization mass spectra (HR-ESI-MS), optical rotatory dispersion (ORD) and electronic circular dichroism (ECD). All of them were assessed for their antioxidant activities through ABTS, DPPH and PTIO methodologies, and evaluated for inhibitory activities against two enzymes (mushroom tyrosinase and acetylcholinesterase). As a result, compounds 3–6, 10 and 13 exhibited evident antioxidant activities. Meanwhile, compounds 5, 10 and 13 showed the most potent tyrosinase inhibitory activities, with IC₅₀ of 0.64, 0.65 and 0.59 mM, and compared with the positive control of 0.63 mM (kojic acid). In the initial concentration of 1 mg/mL, compounds 3, 5 and 6 demonstrated moderate inhibitory activities against acetylcholinesterase with 85.27 ± 0.06%, 83.65 ± 0.48% and 82.21 ± 0.09%, respectively, compared with the positive control of 91.17 ± 0.23% (donepezil). These bioactive components could be promising antioxidants, tyrosinase and acetylcholinesterase inhibitors.     

一种Ku波段高效率低磁场同轴相对论返波管

设计了一种工作在Ku波段的低磁场同轴相对论返波管。器件工作在同轴TM01近模式,采用两段式慢波结构构型,在前后段慢波结构中分别主要进行电子束调制与能量提取,以实现高效率工作。通过设计非对称反射腔,引入电子束预调制,进一步加深电子束调制深度,提高了束波互作用效率。通过调节慢波结构中间漂移段长度,进一步优化器件内部场分布,提取段慢波结构处轴向电场强度得到显著增强,器件工作效率可提升至35%。最终,当磁场强度0.6 、二极管电压490 V、二极管电流7.5 A时,获得1.27 GW微波输出,效率约35%,微波频率为14.7 GHz。     

薄壁圆管空间结构的热疲劳可靠性分析

针对薄壁圆管的空间结构,分析其在交变热载荷下的疲劳可靠性问题.为同时考虑由截面平均温度和截面温差造成的疲劳损伤,提出了综合利用剩余强度和疲劳累积损伤模型的分析方法.首先根据疲劳累积损伤相等原理,将截面温差造成的多级扰动应力载荷作用频次等效为平均温度下的常幅应力载荷作用次数,从而将两者产生的热应力载荷统一为一常幅载荷,再利用剩余强度模型基于动态应力强度干涉理论对疲劳可靠度进行分析,得到了结构在综合考虑两种热疲劳状态下的动态可靠度.该方法可避免直接利用疲劳累积损伤理论临界损伤值难以确定的问题,且能体现金属疲劳损伤的真实情况.最后以哈勃望远镜为例,分析了其主梁随疲劳热载荷循环作用下的动态可靠度,得出了一些有意义的结论.