Highly Regio-, Diastereo-, and Enantioselective Synthesis of Tetrahydroazepines and Benzo[b]oxepines through Palladium-Catalyzed [4+3] Cycloaddition Reactions

A novel Pd⁰-catalyzed asymmetric [4+3] annulation reaction of two readily accessible starting materials has been developed for building seven-membered heterocyclic architectures. The potential [3+2] side pathway could be suppressed though fine tuning of the conditions. A broad scope of cycloaddition donors and acceptors participated in the transformation with excellent chemo-, regio-, diastereo-, and enantioselectivtities, leading to valuable tetrahydroazepines and benzo[b]oxepines.     

盲重构频域阵列信号的压缩感知水声目标方位估计

针对复杂海洋环境条件下压缩感知水声目标方位估计性能下降的问题,利用盲源分离能够提高信噪比的优势,提出了一种盲重构频域阵列信号的压缩感知水声目标方位估计方法。首先将阵元域信号通过傅里叶变换方法得到多个子带阵列信号;然后对各个子带阵列信号进行复数域盲源分离得到子带解混矩阵和子带分离信号估计,并对子带分离信号进行属性分析和处理;再根据处理后的子带分离信号和子带解混矩阵重构子带阵列信号,对重构的子带阵列信号采用频域压缩感知方法进行空间谱估计,得到各个子带的空间谱;最后将各子带得到的空间谱进行求和,搜索求和后空间谱的峰值则可实现目标方位估计。模拟器数据和海上实测数据验证结果表明,同等条件下该方法的目标检测能力优于经典的最小方差无失真响应(Minimum Variance Distortionless Response,MVDR)方法、频域压缩感知(Compressed Sensing,CS)方法、盲源分离(Blind Source Separation,BSS)与MVDR相结合的方法(BSS+MVDR方法),测向精度更高,明显提高了弱目标信号的空间谱能量,增强了声呐检测弱目标的能力。     

高分辨气相色谱/质谱法分析新闻纸和复印纸中的二恶英

随机选择空白的和经过印刷的新闻纸和复印纸,粉碎后用溶剂提取并经多步色谱柱纯化,采用同位素稀释、高分辨气相色谱/高分辨质谱(HRGC/HRMS)联用技术分析了其中的二含量。结果表明:新闻纸中二的总量高于复印纸,但是毒性当量却低于复印纸;经过印刷的新闻纸和复印纸中二的含量均高于空白的新闻纸和复印纸;新闻纸和复印纸中相同二异构体的含量 是不同的。空白的和经过印刷的新闻纸中二毒性当量分别为0.48 ng/kg和0.61 ng/kg,而空白的和经过印刷的复印纸中二恶英毒性当量分别为0.74 ng/kg和0.79     

Ultra-high Tg and ultra-low coefficient of thermal expansion polyimide films based on hydrogen bond interaction

To tolerate high processing temperature during the fabrication of low-temperature polycrystalline silicon thin-film transistors (LTPS–TFT) in flexible OLED devices, the polyimide (PI) films, which are used as substrate, should have ultra-high glass transition temperature (T_g > 450°C) and ultra-low coefficient of thermal expansion (CTE at 0–5 ppm K⁻¹). In this paper, two novel heterocyclic monomers, namely, N,N'-(xanthone-2,7-diyl)bis(4-aminobenzamide) (p-DAXBA) and N,N'-(xanthone-2,7-diyl)bis(3-aminobenzamide) (m-DAXBA), which contain a xanthone moiety, are prepared and polycondensed with pyromellitic dianhydride (PMDA), respectively. PI films (PIa and PIb) with intrinsic high T_g and low CTE are designed from the perspective of rigid conjugate xanthone structure and hydrogen bonding interaction. It is found that the PIa films prepared by p-DAXBA have better linear structure of molecular chains and show relatively higher T_g and lower CTE. The T_g of PIa-40 is greater than 450°C, and CTE can reach as low as 2.7 ppm K⁻¹, tensile strength of 179 MPa, modulus of 5.67 GPa, indicating potential application prospect as a flexible OLED substrate.     

Developing Flexible Quinacridone-Derivatives-Based Photothermal Evaporaters for Solar Steam and Thermoelectric Power Generation

Solar-driven interfacial vaporization by localizing solar-thermal energy conversion to the air−water interface has attracted tremendous attention. In the process of converting solar energy into heat energy, photothermal materials play an essential role. Herein, a flexible solar-thermal material di-cyan substituted 5,12-dibutylquinacridone (DCN−4CQA)@Paper was developed by coating photothermal quinacridone derivatives on the cellulose paper. The DCN−4CQA@Paper combines desired chemical and physical properties, broadband light-absorbing, and shape-conforming abilities that render efficient photothermic vaporization. Notably, synergetic coupling of solar-steam and solar-electricity technologies by integrating DCN−4CQA@Paper and the thermoelectric devices is realized without trade-offs, highlighting the practical consideration toward more impactful solar heat exploitation. Such solar distillation and low-grade heat-to-electricity generation functions can provide potential opportunities for fresh water and electricity supply in off-grid or remote areas.     

Reverse Thinking of the Aggregation-Induced Emission Principle: Amplifying Molecular Motions to Boost Photothermal Efficiency of Nanofibers**

Using reverse thinking of the aggregation-induced emission (AIE) principle, we demonstrate an ingenious and universal protocol for amplifying molecular motions to boost photothermal efficiency of fibers. Core–shell nanofibers having the olive oil solution of AIE-active molecules as the core surrounded by PVDF-HFP shell were constructed by coaxial electrospinning. The molecularly dissolved state of AIE-active molecules allows them to freely rotate and/or vibrate in nanofibers upon photoexcitation and thus significantly elevates the proportion of non-radiative energy dissipation, affording impressive heat-generating efficiency. Photothermal evaluation shows that the core–shell nanofibers with excellent durability can reach up to 22.36 % of photothermal conversion efficiency, which is 26-fold as the non-core–shell counterpart. Such a core–shell fiber can be used for photothermal textiles and solar steam generation induced by natural sunlight with green and carbon-zero emission.     

Adsorption Site Regulation to Guide Atomic Design of Ni–Ga Catalysts for Acetylene Semi‐Hydrogenation

Atomic regulation of metal catalysts has emerged as an intriguing yet challenging strategy to boost product selectivity. Here, we report a density functional theory‐guided atomic design strategy for the fabrication of a NiGa intermetallic catalyst with completely isolated Ni sites to optimize acetylene semi‐hydrogenation processes. Such Ni sites show not only preferential acetylene π‐adsorption, but also enhanced ethylene desorption. The characteristics of the Ni sites are confirmed by multiple characterization techniques, including aberration‐corrected high‐resolution scanning transmission electron microscopy and X‐ray absorption spectrometry measurements. The superior performance is also confirmed experimentally against a Ni₅Ga₃ intermetallic catalyst with partially isolated Ni sites and against a Ni catalyst with multi‐atomic ensemble Ni sites. Accordingly, the NiGa intermetallic catalyst with the completely isolated Ni sites shows significantly enhanced selectivity to ethylene and suppressed coke formation.     

Periodic solution of a two-species competitive system with toxicant and birth pulse

In this paper, we study the existence of positive periodic solution of two-species competitive system with toxicant and birth pulse. A set of easily verifiable sufficient conditions are derived for the existence of at least one positive periodic solution of the above system by using the method of coincidence degree. Numerical simulations are also presented to illustrate the feasibility of our main results.     

The photodetector of Ge nanocrystals/Si for 1.55 μm operation deposited by pulsed laser deposition

The photodetector properties of a Ge nanocrystals detector fabricated by pulsed laser deposition and in situ rapid thermal annealing treatment at 600 °C have been studied. Strong optical absorption and photocurrent response of the detector are measured in the wavelength range 1.3-1.55 μm. The detector possesses a low dark current of 61.4 nA and a photocurrent responsivity of 56 mA/W at the reverse bias 5 V. The external quantum efficiency at 1.55 μm is estimated to be 15%. The stop wavelength of absorption spectra extends to 1.65 μm. It indicates that these kind of Ge nanocrystals devices can be used as a 1.3-1.55 μm near infrared detector.     

奇异二阶拟线性椭圆型方程Dirichlet问题（Ⅲ）

本文应用摄动方法、上下解方法、截断函数方法，得到了一类带奇异项的二阶拟线性椭圆型方程Ｄｉｒｉｃｈｌｅｔ问题正解的存在性和正则性，发展了文献［１］－［７］的相应工作．