Lattice Distortion in Hollow Multi-Shelled Structures for Efficient Visible-Light CO2 Reduction with a SnS2/SnO2 Junction

Precise control of the micro-/nanostructures of nanomaterials, such as hollow multi-shelled structures (HoMSs), has shown its great advantages in various applications. Now, the crystal structure of building blocks of HoMSs are controlled by introducing the lattice distortion in HoMSs, for the first time. The lattice distortion located at the nanoscale interface of SnS₂/SnO₂ can provide additional active sites, which not only provide the catalytic activity under visible light but also improve the separation of photoexcited electron–hole pairs. Combined with the efficient light utilization, the natural advantage of HoMSs, a record catalytic activity was achieved in solid–gas system for CO₂ reduction, with an excellent stability and 100 % CO selectivity without using any sensitizers or noble metals.     

Crystallization-Induced Reversal from Dark to Bright Excited States for Construction of Solid-Emission-Tunable Squaraines

Squaraines (SQs) with tunable emission in the solid state is of great importance for various demands; however a remaining challenge is emission quenching upon aggregation. Herein, a unique SQ, named as CIEE-SQ, is designed to exhibit strong emission in crystal, undergoing crystallization-induced reverse from dark ¹(n+σ,π*) to bright ¹(π,π*) excited states. Such an excited state of CIEE-SQ can be subtly tuned by molecular conformation changes during the unexpected temperature-triggered single-crystal to single-crystal (SCSC) reversible transformation. Furthermore, co-crystallization between CIEE-SQ and chloroform largely stabilize the ¹(π,π*) state, enhancing the transition dipole moment and decreasing the reorganization energy to boost the fluorescence, which is promising in data encryption and decryption.     

Cascade One‐Pot Synthesis of Orange‐Red‐Fluorescent Polycyclic Cinnolino[2,3‐f]phenanthridin‐9‐ium Salts by Palladium(II)‐Catalyzed C−H Bond Activation of 2‐Azobiaryl Compounds and Alkenes

Quaternary ammonium salts were synthesized in moderate to good yields through double oxidative C?H bond activation on azobenzenes. The mechanism of the highly regioselective reaction of 2‐azobiaryls with alkenes to give orange‐red‐fluorescent cinnolino[2,3‐f]phenanthridin‐9‐ium salts and 15H‐cinnolino[2,3‐f]phenanthridin‐9‐ium‐10‐ide is proposed to involve ortho C?H olefination of the 2‐azobiaryl compound with the alkene, intramolecular aza‐Michael addition, concerted metalation–deprotonation (CMD), reductive elimination, and oxidation.     

Orthogonal Cationic and Radical RAFT Polymerizations to Prepare Bottlebrush Polymers

An orthogonal combination of cationic and radical RAFT polymerizations is used to synthesize bottlebrush polymers using two distinct RAFT agents. Selective consumption of the first RAFT agent is used to control the cationic RAFT polymerization of a vinyl ether monomer bearing a secondary dormant RAFT agent, which subsequently allows side‐chain polymers to be grafted from the pendant RAFT agent by a radical‐mediated RAFT polymerization of a different monomer, thus completing the synthesis of bottlebrush polymers. The high efficiency and selectivity of the cationic and radical RAFT polymerizations allow both polymerizations to be conducted in one‐pot tandem without intermediate purification.     

A Molecular Thermochromic Ferroelectric

Molecular ferroelectrics have attracted considerable interests because of their easy and environmentally friendly processing, low acoustical impedance and mechanical flexibility. Herein, a molecular thermochromic ferroelectric, N,N′‐dimethyl‐1,4‐diazoniabicyclo[2.2.2]octonium tetrachlorocuprate(II) ([DMe‐DABCO]CuCl₄) is reported, which shows both excellent ferroelectricity and intriguing thermochromism. [DMe‐DABCO]CuCl₄ undergoes a ferroelectric phase transition from Pca2₁ to Pbcm at a significantly high Curie temperature of 413 K, accompanied by a color change from yellow to red that is due to the remarkable deformation of [CuCl₄]^2? tetrahedron, where the ferroelectric and paraelectric phases correspond to yellow and red, respectively. Combined with multiple bistable physical properties, [DMe‐DABCO]CuCl₄ would be a promising candidate for next‐generation smart devices, and should inspire further exploration of multifunctional molecular ferroelectrics.     

Real‐Time Atomic‐Scale Visualization of Reversible Copper Surface Activation during the CO Oxidation Reaction

By using in situ aberration‐corrected environmental transmission electron microscopy, for the first time at atomic level, the dynamic evolution of the Cu surface is captured during CO oxidation. Under reaction conditions, the Cu surface is activated, typically involving 2–3 atomic layers with the formation of a reversible metastable phase that only exists during catalytic reactions. The distinctive role of CO and O₂ in the surface activation is revealed, which features CO exposure to lead to surface roughening and consequently formation of low‐coordinated Cu atoms, while O₂ exposure induces a quasi‐crystalline CuOx phase. Supported by DFT calculations, it is shown that crystalline CuOx reversibly transforms into the amorphous phase, acting as an active species to facilitate the interaction of gas reactants and catalyzing CO oxidation.     

简单有效的运动汽车投影阴影分割算法

在实时的车型识别系统中,由于光照的影响,需要一种简单快速有效的方法将汽车车体与其阴影分割开。利用阴影的光谱属性,同时根据阴影的几何特征及阴影区域内的点和汽车的空间位置、形状等相关特点,提出一种基于小波变换多分辨率特性的阴影分割算法,该算法能有效地分割出阴影与目标之间的分界线。先利用阴影的光谱属性对阴影进行粗分割,然后利用小波变换的多尺度性对候选阴影点进行特征提取,从而获取最后的阴影分界线。该方法不需要事先确定光源的方向、车体的彩色信息和背景纹理信息,能有效地分割任何颜色、任何背景纹理下、任何光源方向下的运动汽车投影阴影。实验表明,该方法定位准确,处理速度快,抗噪能力强,为进一步的车型识别提供基础。     

在化学实验课中运用剖析-比较-发散实验教学法的探讨

分析了几种化学课的教学目的和特点,提出并论述了剖析-比较-发散实验教学法的具体内容和实施步骤,并对研究探讨这种教学法的必要性作了说明。     

宽频带激光自由空间传输的调制特性研究

基于惠更斯-菲涅耳衍射积分公式,研究了宽带光束在菲涅耳衍射区的自由空间传输特性,得到宽带光束传输的调制深度与光束带宽Δλ及菲涅耳数F的变化关系。结果表明:一定的带宽对光束的均匀性有适当的改善;当光束的带宽Δλ<2λ0/F时,带宽越大,光束越均匀;当带宽满足条件Δλ=2λ0/F时,菲涅耳衍射完全消失;在一定的菲涅耳数范围内,宽带光束的调制深度随菲涅耳数振荡变化,振荡曲线的主极大值和次极大值分别出现在菲涅耳数为奇数和偶数处,而极小值则出现在菲涅耳数F=2k±1/3(k=1,2,3,…)处,在极小值处光束的均匀性最好。     

Magnetic Phase Diagram of the MnxFe2−xP1−ySiy System

The phase diagram of the magnetocaloric Mn_xFe_2−xP_1−ySi_y quaternary compounds was established by characterising the structure, thermal and magnetic properties in a wide range of compositions (for a Mn fraction of 0.3 ≤ x < 2.0 and a Si fraction of 0.33 ≤ y ≤ 0.60). The highest ferromagnetic transition temperature (Mn_0.3Fe_1.7P_0.6Si_0.4, T_C = 470 K) is found for low Mn and high Si contents, while the lowest is found for low Fe and Si contents (Mn_1.7Fe_0.3P_0.6Si_0.4, T_C = 65 K) in the Mn_xFe_2−xP_1−ySi_y phase diagram. The largest hysteresis (91 K) was observed for a metal ratio close to Fe:Mn = 1:1 (corresponding to x = 0.9, y = 0.33). Both Mn-rich with high Si and Fe-rich samples with low Si concentration were found to show low hysteresis (≤2 K). These compositions with a low hysteresis form promising candidate materials for thermomagnetic applications.