Effects of redox-active interlayer anions on the oxygen evolution reactivity of NiFe-layered double hydroxide nanosheets

Nickel-iron layered double hydroxide (NiFe-LDH) nanosheets have shown optimal oxygen evolution reaction (OER) performance; however, the role of the intercalated ions in the OER activity remains unclear. In this work, we show that the activity of the NiFe-LDHs can be tailored by the intercalated anions with different redox potentials. The intercalation of anions with low redox potential (high reducing ability), such as hypophosphites, leads to NiFe-LDHs with low OER overpotential of 240 mV and a small Tafel slope of 36.9 mV/dec, whereas NiFe-LDHs intercalated with anions of high redox potential (low reducing ability), such as fluorion, show a high overpotential of 370 mV and a Tafel slope of 80.8 mV/dec. The OER activity shows a surprising linear correlation with the standard redox potential. Density functional theory calculations and X-ray photoelectron spectroscopy analysis indicate that the intercalated anions alter the electronic structure of metal atoms which exposed at the surface. Anions with low standard redox potential and strong reducing ability transfer more electrons to the hydroxide layers. This increases the electron density of the surface metal sites and stabilizes their high-valence states, whose formation is known as the critical step prior to the OER process.

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Layered double hydroxides with atomic-scale defects for superior electrocatalysis

Atomic composition tuning and defect engineering are effective strategies toenhance the catalytic performance of multicomponent catalysts by improvingthe synergetic effect; however, it remains challenging to dramatically tune the active sites on multicomponent materials through simultaneous defect engineeringat the atomic scale because of the similarities of the local environment. Herein,using the oxygen evolution reaction (OER) as a probe reaction, we deliberatelyintroduced base-soluble Zn(II) or Al(III) sites into NiFe layered double hydroxides(LDHs), which are one of the best OER catalysts. Then, the Zn(II) or Al(III) siteswere selectively etched to create atomic M(II)/M(III) defects, which dramaticallyenhanced the OER activity. At a current density of 20 mA·cm^?2, only 200 mV overpotential was required to generate M(II) defect-rich NiFe LDHs, which is the best NiFe-based OER catalyst reported to date. Density functional theory(DFT) calculations revealed that the creation of dangling Ni–Fe sites (i.e., unsaturated coordinated Ni–Fe sites) by defect engineering of a Ni–O–Fe site at the atomic scale efficiently lowers the Gibbs free energy of the oxygen evolutionprocess. This defect engineering strategy provides new insights into catalysts atthe atomic scale and should be beneficial for the design of a variety of catalysts.

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Erratum to: Charge transfer in graphene/polymer interfaces for CO2 detection

Nano Research - The order of the authors in the original version of this article was unfortunately incorrect on the first page and the first page of the ESM. Instead of Myungwoo Son1, Yusin Pak1,...     

基于YOLOV4的工件表面质量在线检测方法研究

目的 提升自动化产线上工件表面微小缺陷的检测精度和检测速度。方法 首先,在预处理阶段提出采用CutMix的数据增强方法,增加训练样本的多样性,提高模型的鲁棒性和泛化能力,避免训练模型产生过拟合;使用K–means++聚类算法生成边界候选框,以适应不同尺寸的缺陷,并较早地筛选出更精细的特征。其次,借助CSP Darknet53网络及SPP模块提取输入原始图像的特征,通过训练获得针对工件表面质量的在线检测模型,提升YOLOV4缺陷位置检测及识别的精度。结果 实验结果表明,文中所提出的基于YOLOV4的工件表面质量在线监测方法的预测精度达到97.5%,检测速度达到32.8帧/s,均优于同类的深度学习算法。以贵州某航空工业产品的自动化产线作为实验平台验证了所提方法的可行性和有效性。结论 该方法具备结构简单清晰、自适应性强等优点,检测精度和速度均满足工业场景需求,可以将其用于产品表面质量的在线检测。     

桥梁车辆荷载识别的贝叶斯方法研究

基于贝叶斯推理提出了一种可实现误差模式选择的桥梁车辆荷载识别方法。该方法通过静力影响线构建车辆荷载与实测响应的关系表达式,并建立修正曲面以消除动力效应造成的识别误差。引入与结构响应大小和车速相关的五种误差模式。根据假设的先验分布推导车辆轴重参数的后验分布,以获得车辆荷载的最优估计值和置信区间,并计算各误差模式的后验概率。分别采用简支梁数值算例和某连续梁桥动载试验,对该方法在不同车速工况下的识别精度和可靠性进行了验证。结果表明,修正曲面可以有效消除车辆动力冲击的影响,提高了荷载识别精度;荷载识别结果以置信区间形式呈现,可量化荷载识别结果的不确定性;贝叶斯方法能够识别出最佳误差模式,进一步提升了荷载识别的鲁棒性。     

Subnanosecond switching, plasma electrode pockels cell for high-contrast imaging with partially coherent light

A high-contrast optical switch for imaging partially coherent light (~150 times the diffraction limit) requires that it have a large angular acceptance. We describe the development of a high-speed Pockels cell that uses a thin crystal to simultaneously achieve high-contrast (greater than 1800:1) and large-angular acceptance (greater than 7 mrad for a 5-mm aperture). A KD*P crystal was used in a longitudinal-mode configuration with plasma discharges forming low-resistance, high optical transmission electrodes to couple the switching voltage. Rise times of the switched optical pulse of the order of 500 ps were observed. Characterization of the device in the near and far fields was also performed.     

Inviscid melt-spun high-temperature alumina-magnesia fibres

Al₂O₃-MgO (AM) fibres containing 98.16 wt% Al₂O₃ and 1.84 wt% MgO, were produced via inviscid melt spinning. By using scanning electron microscopy it was found that the as-spun AM fibres were hollow and their surfaces were very rough. The X-ray diffraction pattern of the as-spun AM fibre showed -Al₂O₃ as a major phase and -Al₂O₃ as a minor phase. The DTA curve of the as-spun AM fibre showed a single endothermic peak representing the phase transformation of -Al₂O₃ to -Al₂O₃. This phase transformation was readily confirmed by analysing the X-ray diffraction pattern of heat-treated AM fibres.     

Preparation of nanometre size oxide particles using filter expansion aerosol generator

Crystalline zinc oxide particles of nanometre size (< 20 nm) particles were produced from a zinc acetate solution by using a filter expansion aerosol generator (FEAG). The FEAG is an aerosol generator that is operated at 60 torr reactor pressure and produces droplets of around 2 m. The shape of the particles produced by the FEAG were distinctively different from those produced by the ultrasonic spray source (USS). Results from scanning electron microscopy (SEM) and X-ray diffractometry (XRD) indicated that crystalline zinc oxide particles of nanometre size were produced at 600 °C in 0.02 s residence time. Weight loss of these particles, determined by thermogravimetric analysis (TGA), was 3 wt%. Based on the morphology change as a function of the reactor temperature and solute concentration, we proposed that the nanometre particles were formed by uniform precipitation at the drying stage and decomposition followed by disintegration into nanometre particles. It was also shown that exothermic decomposition of the solute was not required for the disintegration of the primary particles in the FEAG process. This result opened up an opportunity for producing carbon-free nanometre particles from nitrate salts by using the FEAG.     

The effect of additives on the crystallization and sintering of 2MgO-2Al2O3-5SiO2 glass-ceramics

Crystallization and sintering behaviour of three cordierite (2MgO-2Al₂O₃-5SiO₂) glasses containing different amount of additives were investigated and compared by using differential thermal analysis (DTA), X-ray diffraction (XRD), scanning electron microscopy (SEM), and the Archimedes method. The stoichiometric 2MgO-2Al₂O₃-5SiO₂ (MAS) glass and the 2MgO-2Al₂O₃-5SiO₂ glass containing 3 wt% of B₂O₃ and 3 wt% of P₂O₅ (MASBP) showed two exotherms (one for -cordierite formation from a glass and the other for -cordierite formation from the -cordierite phase), whereas the 2MgO-2Al₂O₃-5SiO₂ glass containing 2 wt % of B₂O₃, 2 wt% of P₂O₅, and 2 wt % of TiO₂ (MASBPT) showed only a single exotherm representing -cordierite formation. By using Kissinger, Augis-Bennett, Ozawa, and modified Kissinger methods, the activation energy values for -cordierite formation in the MASBP and MASBPT glasses were determined as 310±6 and 326±13 kJ mol^–1, respectively, whereas that in the MAS glass was determined as 868±5 kJ mol^–1. The MASBPT glass showed the lowest peak temperature value for -cordierite formation (980 °C) amongst the three glasses. Both the MASBP and MASBPT glasses showed excellent sintering behaviour (> 99.7% of theoretical density).     

智能CAI软件生成平台

本文概要介绍“智能ＣＡＩ软件生成平台”的研制目标,设计思想,主要功能和技术特点及其实现。