Electrochemical reduction of CO2: Two- or three-electrode configuration

Electrocatalytical conversion of CO₂ into various chemicals like hydrocarbons and CO is regarded as a promising approach to mitigate carbon emission and, meanwhile, to provide sustainable energy and value-added chemicals. Two different reactors are used in this work. One is based upon the two-electrode configuration powered by a DC power supply or Si solar cell, which is suitable for practical applications. Another is three-electrode one powered by a potentiostat, which is feasible to study the electrode performance. Polycrystalline Cu electrode is used as the cathode, and hematite is the anode. Performance of CO₂ reduction using the two- and three-electrode configurations is studied by measuring electrode potential, cell voltage, current density, Faradaic efficiency, and reduction selectivity of CO₂. Cu cathode used here exhibits a low overpotential for CO₂ reduction, specifically for the cell with two-electrode configuration. No obvious difference can be observed between the two types of configurations at a low bias like −0.3 and −0.4 V; while the reactor with two-electrode configuration exhibits better performance at a high bias like −0.8 V than the one with three-electrode configuration. Thus, the reactors with two-electrode configuration are desirable for practical applications, specifically considering solar cells can be used as the power source to provide green and sustainable energy.     

溶解氧变化对阴极极化下10Ni5CrMo钢氢脆敏感性的影响

摘要：为研究溶解氧质量浓度对10Ni5CrMo钢在阴极极化条件下氢脆敏感性影响规律，对10Ni5CrMo钢进行了阴极极化下的电化学交流阻抗谱测试﹑并采用慢应变速率拉伸实验和断口分析方法研究了海水中溶解氧质量浓度变化和不同阴极极化下10Ni5CrMo钢的氢脆敏感性。结果表明：溶解氧质量浓度变化对10Ni5CrMo钢强度几乎没有影响；同一溶解氧质量浓度下，随极化电位负移，断裂时间、伸长率、断面收缩率明显降低，氢脆系数增加，氢脆敏感性显著提高，极化电位达到-1000mV时，氢脆系数已超过安全区允许的最高值25%，进入危险区；同一极化电位下，随着海水中溶解氧质量浓度减少，材料塑性变差，断裂时间、伸长率和断面收缩率不断降低，氢脆系数增加，氢脆敏感性提高。     

Activation of LSCF–YSZ interface by cobalt migration during electrolysis operation in solid oxide electrolysis cells

High-temperature water electrolysis through solid oxide electrolysis cells (SOEC) will play a key role in building a hydrogen economy in the future. However, the delamination between the air electrode and the electrolyte remains a critical issue to be addressed. Previously, it was hypothesized that Co migration may improve the catalytic activity of the SrZrO₃ second phase at the LSCF-YSZ interface, eventually leading to the delamination. In this work, the LSCF-YSZ interfaces sintered at different temperatures were examined in detail. The activation behaviors of the LSCF electrodes upon application with electrolysis current were characterized under different conditions. Further, samples containing purposely added SrZrO₃ interlayer with and without cobalt were fabricated and compared. The activation process is less significant for the sample with cobalt-added SrZrO₃ interlayer than the sample with pure SrZrO₃ layer, supporting the hypothesis that Co migration may lead to the activation behavior.     

Polarization and coherence in the Hanbury Brown–Twiss effect

We study the correlation of intensity fluctuations in random electromagnetic beams, the so-called Hanbury Brown–Twiss effect (HBT). We show that not just the state of coherence of the source, but also its state of polarization has a strong influence on the far-zone correlations. Different types of sources are found to have different upper bounds for the normalized HBT coefficient.     

A Minimalist Single-Layer Metasurface for Arbitrary and Full Control of Vector Vortex Beams

Vector vortex beams (VVBs) possess ubiquitous applications from particle trapping to quantum information. Recently, the bulky optical devices for generating VVBs have been miniaturized by using metasurfaces. Nevertheless, it is quite challenging for the metasurface-generated VVBs to possess arbitrary polarization and phase distributions. More critical is that the VVBs' annular intensity profiles demonstrated hitherto are dependent on topological charges and are hence not perfect, posing difficulties in spatially shared co-propagation of multiple vortex beams. Here, a single-layer metasurface to address all those aforementioned challenges in one go is proposed, which consists of two identical crystal-silicon nanoblocks with varying positions and rotation angles (i.e., four geometric parameters throughout). Those four geometric parameters are found to be adequate for independent and arbitrary control of the amplitude, phase, and polarization of light. Perfect VVBs with arbitrary polarization and phase distributions are successfully generated, and the constant intensity profiles independent of their topological charges and polarization orders are demonstrated. The proposed strategy casts a distinct perception that a minimalist design of just one single-layer metasurface can empower such robust and versatile control of VVBs. That provides promising opportunities for generating more complex vortex field for advanced applications in structural light, optical micromanipulation, and data communication.     

质子交换膜燃料电池电化学阻抗谱弛豫时间分布研究

电化学阻抗谱技术能够获取燃料电池不同频率阻抗，但对阻抗的构成缺乏进一步解析，难以直接构建精准的等效电路模型进行阻抗拟合分析，而弛豫时间分布（Distribution of relaxation time，DRT）方法不需要定义特定的等效电路模型，即可解析燃料电池不同时间常数的极化过程。针对实验室用质子交换膜燃料电池，在不同运行条件下对其进行阻抗谱测量，并通过Kramers-Kronig关系验证所记录阻抗数据的质量。基于DRT分析方法，系统地解释阻抗谱中各频段阻抗对应的物理或化学意义。研究表明，该电池的电化学阻抗谱主要由3个不同时间常数频段的极化阻抗构成，通过与运行条件相关性的系统分析，确定低频段阻抗为氧气在多孔介质中的传输阻碍，中频段阻抗为与氧还原反应有关的电荷传递阻碍，中高频段阻抗为阴极催化剂层中的质子传输阻碍。为进一步确定DRT分析结果的合理性，采用等效电路模型拟合测量的阻抗数据，辨识的电阻元件参数变化趋势与DRT分析结果一致。     

海面油膜的偏振反射特性仿真实验

为了给海面溢油污染识别检测提供理论基础,根据菲涅尔反射公式的偏振反射系数,结合偏振双向反射率因子和粗糙海面的概率密度分布函数,建立了完善的pBRDF模型,仿真在不同太阳入射角度、不同探测器观测角度以及不同海面风速风向等条件下海水和油膜的偏振反射分布函数。结果表明:海水和油膜太阳天顶角为53°和56°时P偏振反射率分别为1.0×10^-5和2.5×10^-5,S偏振反射率随着太阳天顶角的增加而增加;海面风速越大偏振反射率峰值越小;海面风向只改变pBRDF的空间位置;海水和油膜线偏振度空间分布有明显差异。搭建实验平台相机以40°拍摄时,得出海水和油膜的线偏振度分别在0.2~0.4, 0.5~0.7之间,同时表明利用偏振探测获取目标场景的偏振度和偏振角图可提高图像质量。     

Imidazolium-Functionalized Diacetylene Amphiphiles: Strike a Lighter and Wear Polaroid Glasses to Decipher the Secret Code

The development of smart inks that change color and transparency in response to external stimuli is very important for various fields, from modern art to safety and anticounterfeiting technology. A uniaxially oriented diacetylene thin film on a macroscopic area is obtained by coating, self-assembling and topochemical photopolymerizing of imidazolium-functionalized diacetylenes (M-DA and T-DA) and 4,6-decadiyne ink (70 wt%:20 wt%:10 wt%) exhibiting a lyotropic smectic A liquid-crystalline phase at room temperature. The color and transparency of letters and symbols written with the DA-based secret inks change reversibly from blue to red as well as from colorless transparent to black opaque depending on the temperature and polarization axis. A secret code written with thermoresponsive and polarization-dependent secret inks consisting of imidazolium-functionalized diacetylenes is successfully deciphered by wearing polaroid glasses and holding a burning torch.     

Large domain-wall currents in epitaxial Au/BiFeO3/SrRuO3 thin-film capacitors with modulated oxygen vacancy and wall densities

Large domain wall (DW) conductivity in an insulating ferroelectric plays an important role in the future nanosensors and nonvolatile memories. However, the wall current was usually too small to drive high-speed memory circuits and other agile nanodevices requiring high output-powers. Here, a large domain-wall current of 67.8 μA in a high on/off ratio of ~4460 was observed in an epitaxial Au/BiFeO₃/SrRuO₃ thin-film capacitor with the minimized oxygen vacancy concentration. The studies from read current-write voltage hysteresis loops and piezo-response force microscope images consistently showed remaining of partially unswitched domains after application of an opposite poling voltage that increased domain wall density and wall current greatly. A theoretical model was proposed to explain the large wall current. According to this model, the domain reversal occurs with the appearance of head-to-head and tail-to-tail 180° domain walls (DWs), resulting in the formation of highly conductive wall paths. As the applied voltage increased, the domain-wall number increased to enhance the on-state current, in agreement with the measurements of current-voltage curves. This work paves a way to modulate DW currents within epitaxial Au/BiFeO₃/SrRuO₃ thin-film capacitors through the optimization of both oxygen vacancy and domain wall densities to achieve large output powers of modern domain-wall nanodevices.