FeO/Pt(111)与FeO2/Pt(111)的几何、电子结构及表面氧活性的第一性原理研究

采用密度泛函理论系统研究了超薄氧化物膜/金属体系FeO/Pt和FeO₂/Pt及其表面不同区域(FCC,HCP和TOP)的几何结构、电子性质及氧的活性.研究发现,表面O-Fe高度差δ_z作为一个重要的特征结构参数直接影响局域表面静电势和表面氧的结合能: δ_z越大,静电势越大,氧的结合能越弱.计算发现,在FeO/Pt体系中,δ_z顺序为FCC > HCP > TOP,而FeO₂/Pt中是FCC > TOP > HCP.此外,在FeO/Pt中,电荷转移方向是从氧化物膜到衬底,Fe的表观价态为+2.36,表面功函较纯Pt(111)的变化可忽略; 而FeO₂/Pt中,电荷转移的方向是从衬底到氧化物,Fe的表观价态为+2.95,表面功函较纯Pt增加1.24 eV.进一步分析了电荷转移和表面偶极对电子性质的作用机制.这些研究结果对于认识超薄氧化物薄膜对表面几何结构、电子性质、表面氧活性的调制具有重要的启示意义.     

钡钨阴极优化与热电子发射性能

分别从基体和铝酸盐两方面优化了钡钨阴极.在基体方面,首先采用窄粒度钨粉结合放电等离子体烧结获得了孔径分布窄的基体;再利用射频等离子体球化技术制备了球形钨粉,采用球形钨粉制备了多孔基体,获得了孔通道光滑、内孔连通性好、孔径分布更加窄的基体.与窄粒度钨粉基体相比,球形钨粉制备的阴极,空间电荷限制区的斜率由1.25增加至1.37,发射均匀性得到提高,拐点电流密度由6.6 A·cm^–2增至6.96 A·cm^–2.在此基础上,采用液相法改善了铝酸盐物相组成,发现空间电荷限制区的斜率增加至1.44,拐点电流密度增加至21.2 A·cm^–2.通过理论计算对钡钨阴极发射的物理本质进行了研究,发现钡钨阴极发射规律遵循偶极子理论.     

速度限制对交通流的影响

运用元胞自动机模型研究单车道路面上设立限速区对交通流的影响.计算机模拟结果显示,在交通流与密度的基本图中存在饱和交通流量,其大小取决于限速区的最大速度.限速区的设立导致不同相的分离.在确定性的模型中,当车辆密度较低时,存在两种不同的自由流相;而当车辆密度较高时,出现最大交通流相和自由流相.在随机模型中,车辆密度较高时,出现最大交通流相-堵塞相-自由流.对交通流以及临界密度等量给出一些解析结果.     

Fe2O3/LaNiO3载氧体在化学链制氢中应用的可行性研究

采用柠檬酸络合法制备了Fe2O3/LaNiO3复合氧化物,将该氧化物作为化学链制氢反应的载氧体,对燃料反应器温度、蒸汽反应器温度、剂烷比(Fe2O3/CH4)、进水量等工艺条件进行了考察。实验结果表明:燃料反应器温度达到800℃以上甲烷都可以全部转化,燃料反应器温度、剂烷比和进水量对氢气产量影响比较大。在燃料反应器温度为850℃、蒸汽反应器温度为900℃、常压、剂烷比为2/1,进水量为0.1 mL时对载氧体进行连续60次氧化-还原循环,结果是前57次循环载氧体稳定性非常好,从第58次循环开始氢气产量迅速下降,结合XRD和TEM表征发现载氧体在高温下连续进行氧化-还原反应,导致部分载氧体结构发生分解,失去了原来结构具有很强的储氧-释氧能力,导致氢气产量下降,稳定性变差。     

Noise reduction in LOS wind velocity of Doppler lidar using discrete wavelet analysis

The line of sight (LOS) wind velocity can be determined from the incoherent Doppler lidar backscattering signals. Noise and interference in the measurement greatly degrade the inversion accuracy. In this paper, we apply the discrete wavelet denoising method by using biorthogonal wavelets and adopt a distance-dependent thresholds algorithm to improve the accuracy of wind velocity measurement by incoherent Doppler lidar. The noisy simulation data are processed and compared with the true LOS wind velocity. The results are compared by the evaluation of both the standard deviation and correlation coefficient. The results suggest that wavelet denoising with distance-dependent thresholds can considerably reduce the noise and interfering turbulence for wind lidar measurement.     

Probing the improved stability for high nickel cathode via dual-element modification in lithium-ion

One of the major hurdles of nickel-rich cathode materials for lithium-ion batteries is the low cycling stability, especially at high temperature and high voltage, originating from severe structural degradation, which makes this class of cathode less practical. Herein, we compared the effect of single and dual ions on electrochemical performance of high nickel (LiNi_0.88Mn_0.03Co_0.09O₂, NMC) cathode material in different temperatures and voltage ranges. The addition of a few amounts of tantalum (0.2 wt%) and boron (0.05 wt%) lead to improved electrochemical performance. The co-modified LiNi_0.88Mn_0.03Co_0.09O₂ displays an initial discharge capacity of 234.9 mAh/g at 0.1 C and retained 208 mAh/g at 1 C after 100 cycles at 45 ℃, which corresponds to a capacity retention of 88.5%, compared to the initial discharge capacity of 234.1 mAh/g and retained capacity of 200.5 mAh/g (85.6%). The enhanced capacity retention is attributed to the synergetic effect of foreign elements by acting as a surface structural stabilizer without sacrificing specific capacity.     

Structural evolution of the intruder band in ~(118)Sn

Excited states of the positive-parity intruder band in ¹¹⁸Sn have been studied via the ¹¹⁶Cd(⁷Li, 1p4n) reaction at ⁷Li energy of 48 MeV using techniques of in-beam γ-ray spectroscopy. This intruder band has been observed up to 7187 keV with spin (16⁺). The structural evolution of this intruder band with increasing angular momentum has been discussed in terms of the aligned angular momentum and the ratio of the E-Gamma Over Spin (E-GOS) curve.     

氧气气氛下Pt3Ni(111)表面结构变化的从头算原子热力学研究

采用从头算原子热力学方法系统研究了Ni-rich和Pt-rich条件下Pt₃Ni(111)在不同偏析、表面化学吸附氧覆盖度下560个可能结构的相对稳定性,构建了氧气气氛下Pt₃Ni(111)表面结构演化、直至满覆盖化学吸附氧的热力学相图.结果表明,随着氧的化学势的升高,在热力学上仅出现两类稳定的结构,主要包括没有化学吸附氧的干净Pt-skin表面,以及在很低氧的化学势下就形成的含有化学吸附氧的Ni-skin表面,而有化学吸附氧的PtNi表面合金化的中间结构则处于亚稳态.仔细分析发现,这些结构的形成主要由金属的偏析能、氧与两种金属成键强弱的差别、氧的化学势的高低三个因素共同决定.     

Enhancement of electrochemical performance in lithium-ion battery via tantalum oxide coated nickel-rich cathode materials

Nickel-rich cathode materials are increasingly being applied in commercial lithium-ion batteries to realize higher specific capacity as well as improved energy density. However, low structural stability and rapid capacity decay at high voltage and temperature hinder their rapid large-scale application. Herein, a wet chemical method followed by a post-annealing process is utilized to realize the surface coating of tantalum oxide on LiNi_0.88Mn_0.03Co_0.09O₂, and the electrochemical performance is improved. The modified LiNi_0.88Mn_0.03Co_0.09O₂ displays an initial discharge capacity of ～ 233 mAh/g at 0.1 C and 174 mAh/g at 1 C after 150 cycles in the voltage range of 3.0 V-4.4 V at 45℃, and it also exhibits an enhanced rate capability with 118 mAh/g at 5 C. The excellent performance is due to the introduction of tantalum oxide as a stable and functional layer to protect the surface of LiNi_0.88Mn_0.03Co_0.09O₂, and the surface side reactions and cation mixing are suppressed at the same time without hampering the charge transfer kinetics.     

ORIGINS OF POTASH DEPOSITS IN THE QAIDAM BASIN, CHINA

The Qaidam Basin is a typically continental potash-bearing basin, which is comparatively rare in other countries. The potash deposits are widespread in the Quaternary salt lakes of the mid-western basin. At the same time, there exist many favourable conditions for the formation of potash deposits: (ⅰ)the sufficient source of potassium, (ⅱ) the optimum migration and accumulation processes of potassium, and (ⅲ) proper physico-chemical environments for separating potash salts. Owing to the differences in the supplying conditions for the external water to lake-basin and in the chemical compositions of those salt lake brines, potash deposits of various models and various types were formed.