轨道对称性匹配:MXene基体上的单原子催化以实现优异的氮还原反应

氨作为一种可被植物直接吸收用以合成其他有机物的重要成分,在化学化工及含氮化合物的生产当中起着至关重要的作用.传统工业生产氨气采用Haber-Bosch工艺,将空气中丰富的氮气转化为氨气,但该工艺需要较高的压强和温度来促进氮气分解,因此会消耗大量能源.近年来,电催化反应发展迅速.在电催化工艺中,通过控制操作电位及电解质便可提高生产效率,降低能源消耗.基于这种策略,各种针对能源环境的催化研究应运而生,如二氧化碳还原、水分解反应等.其中,对于氮还原的催化研究尤其是电催化设计领域研究相对较少.研究发现,在电催化剂中,异构掺杂及原子尺度的调控可以极大地影响催化剂的催化活性.其中,单原子催化(SAC)因其在催化活性和催化选择性上的优势受到广泛关注.MXene是一种二维过渡金属碳化物或氮化物,其优异的化学性能和稳定的表面构型可以对单原子起到良好的锚定与支撑作用,是一种更具潜力的单原子催化基体.本文基于上述思想,利用密度泛函第一性原理等模拟软件,设计并研究了以MXene为基体的28种过渡金属单原子催化体系,计算并分析了各SAC@MXene体系对氮还原反应的催化效果,从限制电势、催化路径、反应机制等方面探索了其催化性能.并对体系进行了态密度、晶体轨道哈密顿量、差分电荷密度等电子结构分析,找到了适用于MXene体系的单原子催化设计原则.通过对限制电势的计算表明,Ni@MXene和Co@MXene体系具有很低的限制电势(-0.13和-0.17 V),说明这些体系在较低的启动电压下即可发生氮还原反应.研究发现了一种新型适用于SAC@MXene氮催化体系的酶促-远端反应机制.电子结构分析得到SAC原子与MXene基体的Ti原子在催化过程中存在一种协同作用.态密度及晶体轨道哈密顿量也显示出SAC原子与MXene基体Ti之间的一种轨道对称性匹配关系,揭示了这种协同作用对催化反应的积极作用.计算的氢析出反应(HER)结果也显示,在相同化学环境下,SAC@MXene体系氮还原反应相对于氢析出反应更易发生.     

基于彩色结构光的自由曲面三维重建方法

彩色结构光三维重建过程中,系统的非线性耦合以及待测曲面的拓扑结构等均会对结构光解码产生影响,从而导致调制条纹漏检和颜色码误识别.为解决这一问题,提出一种基于彩色编码结构光的三维重建方法.利用YUV颜色通道对调制条纹进行滤波差分投影处理,通过调制条纹的波形分布提取中心特征线;利用颜色聚类方法精确获取调制条纹的颜色码信息值...     

一类T形树匹配唯一的充要条件

证明：若m∈Ze^ ,则T形树T(1,m,n）匹配唯一当且仅当n≠m,m 3,2m 5.     

A matrix rational Lanczos method for model reduction in large‐scale first‐ and second‐order dynamical systems

In the present paper, we describe an adaptive modified rational global Lanczos algorithm for model‐order reduction problems using multipoint moment matching‐based methods. The major problem of these methods is the selection of some interpolation points. We first propose a modified rational global Lanczos process and then we derive Lanczos‐like equations for the global case. Next, we propose adaptive techniques for choosing the interpolation points. Second‐order dynamical systems are also considered in this paper, and the adaptive modified rational global Lanczos algorithm is applied to an equivalent state space model. Finally, some numerical examples will be given.     

OMIS图像条带噪音消除方法研究

分析了OMIS高光谱图像条带噪音产生的主要原因及条带噪音的特点.提出了两种改进的空域和小波域OMIS条带噪音消除新方法.比较了实验图像和数据.结果表明,两种新方法均具有良好的消除OMIS条带噪音的能力,并能较好地保持图像的纹理细节信息,效果明显优于原有方法.     

Matching subsequences in trees

Given two rooted, labeled trees P and T the tree path subsequence problem is to determine which paths in P are subsequences of which paths in T. Here a path begins at the root and ends at a leaf. In this paper we propose this problem as a useful query primitive for XML data, and provide new algorithms improving the previously best known time and space bounds.     

Addendum to: “Hamilton-laceable bi-powers of locally finite bipartite graphs” [Discrete Math. 345 (2022) 112777]

In this addendum we give a short and easy negative answer to the two questions raised in the original article.     

重力匹配导航的影响模式分析

从重力场匹配导航的改进TERCOM算法入手,针对采样长度、采样间隔以及重力测量误差对匹配结果的影响进行了系统分析,并在此基础上利用海洋年度重力测量数据设计了准实时仿真试验,结果表明:(1)采样长度对匹配结果有重要的影响,采样长度与重力基准图的分辨率比值在10~20之间时,能够获得较好的匹配效果;(2)适当增加采样间隔可以在一定程度上提高匹配的整体精度,但增加了匹配失效的风险,实际应用中采样间隔以2~4 min为宜;(3)重力测量白噪声误差对匹配结果影响相对较大,过大的误差将不能得到有效匹配,水下重力测量误差最好能控制在2 mGal以内。     

Analysis of visual perception of light emitting diode brightness in dense fog with various droplet sizes

Road signs must provide a conspicuous signal to a wide variety of drivers over a broad range of environmental and geometric conditions. Recently, there are an increasing number of applications in which light emitting diodes (LEDs) are used as the light source, including critical transportation signaling. In the presence of fog, the resulting visual signal is disturbed due to light scattering by airborne water droplets. By measuring LED brightness with human spectral sensitivity in various densities and various droplet sizes (10, 30, 50, and 100 μm), it is understood that the particle size distribution (fog droplet size) and density of fog does affect visibility in fog. The colored LEDs that contain a yellow component had high brightness evaluation, blue component had low brightness evaluation in all densities and different droplet sizes. The result in this paper can contribute to air and land traffic safety and the prevention of accidents.     

Confocal Microscopy Studies of Trypsin Immobilization on Porous Glycidyl Methacrylate Beads

The immobilization of trypsin on porous glycidyl methacrylate (GMA–GDMA) beads has been investigated. In particular, the distribution within the beads of trypsin and of dextran used for hydrophilizing the bead surface prior to protein immobilization was investigated with confocal microscopy. For the system investigated, the fluorescence intensity profiles obtained when using borate buffer as an ambient solution displayed a distinct minimum at the center of the beads, irrespective of the observation depth. However, by reduction of the refractive index difference between the solution and the beads through the addition of glucose to the aqueous solution, artifacts relating to optical length differences could be reduced. For both low molecular weight fluorescein isothiocyanate (FITC), FITC-labeled trypsin, and FITC-labeled dextran, an essentially homogeneous distribution throughout the beads was observed. This simple “contrast matching” method seems therefore to be an interesting tool when investigating the distribution of immobilized protein in porous chromatography media.