二氧化硅表面的APTS修饰

3-氨丙基三乙氧基硅烷（APTS）修饰的二氧化硅在生物化学、分析、催化、电子学等领域具有重要的应用前景。本文对近年来APTS修饰二氧化硅的研究进展进行了简要的概述,介绍了APTS修饰二氧化硅的典型方法和APTS修饰层的表征手段,探讨了不同修饰方法可控性及对所形成的APTS层结构及稳定性的影响。     

天然气管道泄漏可调谐二极管激光遥感探测的研究

天然气管道泄漏不仅造成经济损失而且是危险之源。传统的天然气管道泄漏检测技术效率低、速度慢,难以满足实际应用的需要。近年来以近红外二极管激光吸收光谱为基础的光学传感器由于具有灵敏度高、体积小、重量轻和无需维护等优点而得到了广泛的应用。文章以可调谐二极管激光吸收光谱和谐波探测技术为基础进行天然气管道泄漏遥感探测技术的研究,采用二次谐波与一次谐波信号的比值作为系统浓度标定,结果显示浓度与比值之间具有较好的一致性。文章还就不同地形散射体对探测结果的影响进行了测量和分析,实验结果表明二次谐波与一次谐波信号比值标定技术对便携式二极管激光光学测量能够很好的满足实际应用的需要。     

Theoretical study on the catalytic properties of single-atom catalyst stabilised on silicon-doped graphene sheets

ABSTRACT

The stable configurations, electronic structures and catalytic activities of single-atom metal catalyst anchored silicon-doped graphene sheets (3Si-graphene-M, M?=?Ni and Pd) are investigated by using density functional theory calculations. Firstly, the adsorption stability and electronic property of different gas reactants (O₂, CO, 2CO, CO/O₂) on 3Si-graphene-M substrates are comparably analysed. It is found that the coadsorption of O₂/CO or 2CO molecules is more stable than that of the isolated O₂ or CO molecule. Meanwhile, the adsorbed species on 3Si-graphene-Ni sheet are more stable than those on the 3Si-graphene-Pd sheet. Secondly, the possible CO oxidation reactions on the 3Si-graphene-M are investigated through Eley–Rideal (ER), Langmuir–Hinshelwood (LH) and new termolecular Eley–Rideal (TER) mechanisms. Compared with the LH and TER mechanisms, the interaction between 2CO and O₂ molecules (O₂?+?CO → CO₃, CO₃?+?CO → 2CO₂) through ER reactions (< 0.2?eV) are an energetically more favourable. These results provide important reference for understanding the catalytic mechanism for CO oxidation on graphene-based catalyst.     

Influence of Electron–Phonon Interaction on the Lattice Thermal Conductivity in Single-Crystal Si

Lattice thermal conductivity can be reduced by introducing point defect, grain boundary, and nanoscale precipitates to scatter phonons of different wave-lengths, etc. Recently, the effect of electron–phonon (EP) interaction on phonon transport has attracted more and more attention, especially in heavily doped semiconductors. Here the effect of EP interaction in n-type P-doped single-crystal Si has been investigated. The lattice thermal conductivity decreases dramatically with increasing P doping. This reduction on lattice thermal conductivity cannot be explained solely considering point defect scattering. Further, the lattice thermal conductivity can be fitted well by introducing EP interaction into the modified Debye–Callaway model, which demonstrates that the EP interaction can play an important role in reducing lattice thermal conductivity of n-type P-doped single-crystal Si.     

稀土元素(La,Y)掺杂GaN的第一性原理计算

采用基于密度泛函理论的第一性原理赝势平面波方法,对稀土元素La,Y单掺杂和La和Y共掺杂GaN的晶格常数、电子结构及光学性质进行了计算与分析.计算结果表明:掺杂改变了GaN的能带结构,未掺杂和Y掺杂形成导带底和价带顶位于G点的直接带隙半导体,而La掺杂和La和Y共掺杂形成导带底位于G点,价带顶位于Q点的间接带隙半导体.可以通过掺杂元素来调制GaN的禁带宽度和带隙类型,掺杂均提高GaN在低能区的静态介电常数、反射率、折射率,使光子的跃迁强度增大,说明稀土元素La,Y掺杂可有效调制GaN的光电性质.     

Strong Pauli paramagnetic effect in the upper critical field of KCa2Fe4As4F2

Recently, 12442 system of Fe-based superconductors has attracted considerable attention owing to its unique double-Fe As-layer structure. A steep increase in the in-plane upper critical field with cooling has been observed near the superconducting transition temperature, Tc, in KCa2Fe4As4F2 single crystals. Herein, we report a high-field investigation on upper critical field of this material over a wide temperature range, and both out-of-plane(H∥c, Hc2c) and in-plane(H∥ab, Hc2ab ) directions have been measured.A sublinear temperature-dependent behavior is observed for the out-of-plane Hc2c , whereas strong convex curvature with cooling is observed for the in-plane Hc2ab . Such behaviors could not be described by the conventional Werthamer-Helfand-Hohenberg(WHH) model. The data analysis based on the WHH model by considering the spin aspects reveals a large Maki parameter α=9,indicating that the in-plane upper critical field is affected by a very strong Pauli paramagnetic effect.     

Pt(111) 表面上表层 Fe (FeO) 结构和次表层 Fe 结构的可控转变

 利用扫描隧道显微镜 (STM) 和 X 射线光电子能谱 (XPS) 对 Pt(111) 表面制备的 Fe 单层薄膜及其在不同环境气氛条件下的多种结构进行了研究. 在温度为 487 K 的 Pt(111) 表面制备出了完整的 Fe 单层薄膜Fe/Pt(111). 对 Fe/Pt(111) 依次升高温度进行超高真空退火, STM 和 XPS 结果表明退火温度高于 800 K 时, 表面 Fe 原子扩散到次表层区域, 形成次表层 Fe 结构Pt/Fe/Pt(111). Pt/Fe/Pt(111) 在 O2 氧化气氛中经 850 K 退火可转变成表面 FeO 薄膜FeO/Pt(111). FeO/Pt(111) 结构在温和的 H2 还原气氛中 (600 K) 转变成表面 Fe 结构, 进一步的还原处理 (800 K) 则可以重新生成 Pt/Fe/Pt(111). 控制样品的环境气氛在 O2 和 H2 之间切换, 使得表面 Fe (FeO) 和次表面 Fe 可以重复地转变. 本研究实现了多种 Fe-Pt 表面结构的可控制备, 可为合理地设计高效、价廉的催化剂提供借鉴.     

Asymmetric Epoxidation of Terminal Olefins with Binaphthyl Strapped Porphyrin Catalysts: (‐( Stacking Interaction and Steric Effects on the Enantioselectivities

将两种具有相似手性联萘空腔的手性卟啉1b和2b作为催化剂,对苯乙烯衍生物及非芳香烯烃底物进行了催化不对称环氧化反应。应用理论计算方法研究了底物同两种催化剂之间的作用机理;应用1H NMR探讨了催化剂的手性空腔结构;结果表明芳香烯烃同催化剂的手性联萘基团之间的p-p相互作用是决定该类催化剂对映选择性的重要因素,同时催化剂手性结构的立体位阻效应使该类催化剂具有良好的ee值。     

环硅氮烷的合成与应用研究进展(1)——环二硅氮烷

环二硅氮烷是有机硅氮化合物中结构与性能比较特殊的一类化合物,在材料化学及配位化学领域有重要的潜在应用前景.综述了近年来环二硅氮烷的合成方法与应用研究进展.在合成方面,主要分为3条路线,分别由环三硅氮烷锂盐、取代硅胺及六氯化二硅为起始物.在应用领域,介绍了环二硅氮烷的离子开环聚合、等离子聚合、与其它单体的共聚、水解和金属配合物的制备及其在陶瓷、粘合剂和预想的催化剂上的应用.     

高比能锂硫电池正极材料

锂硫电池被认为是最有发展潜力的新型多电子反应的二次电池体系之一.单质硫与锂反应的理论比容量为1675 mA h g?1,质量比能量达2600 W h kg?1,远远高于现行的传统锂离子二次电池材料.同时硫又具有来源丰富、环境友好等优点.然而,仍然有许多问题制约了锂硫电池的发展与广泛应用.本文综述了近年来锂硫电池正极材料的研究进展.