单层和双层二硫化钼化学气相沉积生长的动力学蒙特卡罗模拟研究

Controllable synthesis of MoS₂ with desired number of layers via chemical vapor deposition (CVD) remains challenging. Hence, it is highly desirable to develop a theoretical model that can be used to predict the single- and multilayer growth of MoS₂ quantitatively, and provide guidelines for experimental fabrication. Herein we have established a kinetic Monte Carlo (kMC) model to predict the CVD growth of mono- and bilayer MoS₂. First, we proposed that the growth rates of layer 1 and layer 2 were governed by the distribution of the adatom concentration, and the growth kinetics of compact triangular MoS₂ followed the kink nucleation-propagation mechanism. The adatom concentration was formulated in terms of adatom flux, effective lifetime of adatoms, growth temperature, binding energies, edge energies, and nucleation criterion. The kink nucleation and propagation were determined by energy barriers of the adatom attachments to the zigzag and armchair edges. We then employed an analytic thermodynamic criterion to extract these parameters. Using the calibrated model, we found that the growth rate of layer 2 strongly depended on the size of layer 1 and decreased monotonically with increasing size of layer 1, and might even become prohibited at the maximum size of layer 1. Furthermore, we analyzed the size and morphology evolutions of bilayer MoS₂ at different growth temperatures and adatom fluxes. Throughout the growth processes of bilayer MoS₂, the morphologies of layers 1 and 2 maintained triangular shapes with compact edges, consistent with the kink nucleation-propagation growth mechanism. Our simulations revealed that the growth of bilayer MoS₂ was promoted by increasing the growth temperature or decreasing the adatom flux, which corroborated the experimental observations. The increase in growth temperature led to reduced adatom concentration at the edge of layer 2 in accordance with the adatom concentration far from the edge of layer 2, resulting in a consistent difference in the adatom concentration to promote the growth of bilayer MoS₂. Similarly, the decrease in adatom flux lowered the difference between the adatom concentrations far from the edge and at the edge of layer 1, decelerating the growth of layer 1. The decelerated growth of layer 1 reduced the difference between the adatom concentrations far from the edge and at the edge of layer 2 to zero, permitting the growth of bilayer MoS₂. To guide the experimental synthesis, we constructed a phase diagram to delineate the permitted or prohibited growth of bilayer MoS₂ at different growth temperatures and adatom fluxes. Hence, this work not only unveils the conditions for the growth of mono- and bi-layer MoS₂, but also provides guidelines for controllable synthesis of MoS₂ with the desired number of layers.     

Bismuth-catalyzed methylation and alkylation of quinone derivatives with tert-butyl peroxybenzoate as an oxidant

A bismuth-catalyzed methylation of quinones in the presence of tert-butyl peroxybenzoate (TBPB) was developed via a radical reaction mechanism. Particularly, TBPB was used not only as an efficient oxidant, but also as a green methyl source in such transformation. Moreover, this method could also be efficiently extended to the alkylation of quinones. This reaction tolerated a series of functional groups and prepared a series of derivatives of vitamin K₃ and benzoquinone. Notably, antimalarial parvaquone was synthesized by the reaction.     

粘土矿物参与微生物利用木质素形成矿物-菌体残留物的结构特征研究

粘土矿物在催化木质素形成腐殖质方面具有重要贡献。为有效阐明微生物-木质素-粘土矿物三者间的关系,探明矿物-菌体残留物的结构特征,采用液体摇瓶培养法,以木质素为碳源,通过添加高岭石和蒙脱石,在接种复合菌剂后启动110 d液体培养,期间动态收集矿物-菌体残留物,利用傅里叶红外光谱及扫描电子显微镜技术对其结构特性进行了研究。结果表明：高岭石颗粒边缘多由管状体卷曲而成,在参与微生物利用木质素形成矿物-菌体残留物后,连片状细小颗粒结构进一步团聚,结合更加紧凑,短管状结构增多,但整体仍保持多水高岭石的结构特征;在初始富营养条件下,高岭石能够促进微生物繁衍,使大量菌体聚集于高岭石表面,掩蔽了Si-O和Si-O-Al键,且矿物-菌体残留物中脂族碳结构比例增加;菌体中多糖物质通过含氧官能团与高岭石表面的水化层在多个部位形成氢键,氢键的形成对于高岭石稳定木质素及其降解产物具有重要作用,芳香碳结构比例和多糖类物质含量随培养时间逐渐增加,而后复合菌株对掩蔽在矿物表面的菌体进行二次利用,使高岭石Si-O-Al键重现;蒙脱石多由浑圆的颗粒结构组成,接种微生物可使其表面产生溶蚀,团粒结构遭到破碎;与10 d相比,历经30 d培养所得矿物-菌体残留物中的多糖类物质增多,使原本归属蒙脱石Si-O-Si及Si-O结构的1 034~1 038 cm-1处吸收峰强度增加,而后因多糖类物质与蒙脱石表面羟基发生缔合,又使该处吸收峰强度减弱,同时发生了氢键键合,该作用是蒙脱石-微生物-木质素间相互作用、形成矿物-菌体残留物的主要机制;高岭石在稳定有机碳方面的能力要高于蒙脱石,更易促进HS前体物质的形成。     

高精度欧拉流体弹塑性问题的数值方法研究

将描述固体材料的应力应变关系与欧拉流体动力学方程组耦合求解,通过引入界面捕捉方法描述多物质界面,将带弹塑性的多材料相互作用问题从形式上转化为计算单一材料问题,采用Roe方法近似求解Riemann问题,给出以Godunov方法为基础的二阶精度欧拉弹塑性流动的数值计算方法,适用于计算大变形流动等问题,并通过数值实验进行验证.     

DEM investigation of mixing indices in a ribbon mixer

Mixing index is an important parameter to understand and assess the mixing state in various mixers including ribbon mixers,the typical food processing devices.M...     

A single crystalline porphyrinic titanium metal–organic framework

We successfully assembled the photocatalytic titanium-oxo cluster and photosensitizing porphyrinic linker into a metal–organic framework (MOF), namely PCN-22. A preformed titanium-oxo carboxylate cluster is adopted as the starting material to judiciously control the MOF growth process to afford single crystals. This synthetic method is useful to obtain highly crystalline titanium MOFs, which has been a daunting challenge in this field. Moreover, PCN-22 demonstrated permanent porosity and photocatalytic activities toward alcohol oxidation.     

哈特曼边界层的初级稳定性分析

导电流体在法向外置磁场的作用下,在贴近壁面处会形成哈特曼边界层.哈特曼边界层的稳定性研究对电磁冶金过程和热核聚变反应冷却系统等相关设备的设计和运行都有着十分重要的意义.本文采用非正则模态稳定性分析方法,对两无限大绝缘平行平板内导电流体流动的稳定性进行了研究.通过在时间上迭代求解扰动变量的控制方程组和伴随控制方程组,获得了在磁场作用下初级扰动的增长情况及其空间分布形式,分析了磁场强度对最优扰动增长倍数G_max、最优展向波数β_opt和最优时刻t_opt的影响,并考察了上下两个哈特曼边界层之间的相互作用.结果表明,最优初始扰动的空间分布形式为沿着流场方向的漩涡,关于法向方向对称或者反对称.当哈特曼数Ha较大时(Ha>10),对称漩涡和反对称漩涡形式的初始扰动增长倍数基本相等;上下两个哈特曼边界层可以认为是彼此独立的,不会相互影响,此时最优扰动增长倍数G_max与局部雷诺数R的平方成正比,相应的最优展向波数β_opt和最优时刻t_opt均正比于哈特曼数Ha.当哈特曼数Ha较小时(Ha<10),反对称漩涡形式的初始扰动更为不稳定,其增长倍数大于对称漩涡的增长倍数,且上下两个边界层之间存在着一定的相互作用,并对整个流场的稳定性产生一定的影响.      

火灾升降温模式对高温后钢筋混凝土轴压力学性能影响的试验研究

为研究实际火灾与标准火灾对高温全过程作用后钢筋混凝土力学性能的影响程度,进行了6根大尺寸钢筋混凝土短柱经历不同火灾模式的高温全过程作用后轴压力学性能试验。选择一典型住宅房间,根据欧洲规范得到了模拟火灾温度-时间曲线,利用等效曝火时间方法获得等效标准火灾,考察火灾模式、轴压比对高温全过程作用后钢筋混凝土承载力、刚度和延性的影响规律。试验结果表明:随着轴压比(n0.4)增大,高温后剩余承载力、刚度和延性损伤程度降低;火灾升降温模式影响显著。根据等能量法进行的火灾试验结果和模拟实际火灾试验结果吻合较好,而等面积法过于保守。建议相关规范采用基于能量的等效曝火时间方法进行抗火设计和火灾后剩余力学性能评估。     

A type of biased consensus-based distributed neural network for path planning

In this paper, a unified scheme is proposed for solving the classical shortest path problem and the generalized shortest path problem, which are highly nonlinear. Particularly, the generalized shortest path problem is more complex than the classical shortest path problem since it requires finding a shortest path among the paths from a vertex to all the feasible destination vertices. Different from existing results, inspired by the optimality principle of Bellman’s dynamic programming, we formulate the two types of shortest path problems as linear programs with the decision variables denoting the lengths of possible paths. Then, biased consensus neural networks are adopted to solve the corresponding linear programs in an efficient and distributed manner. Theoretical analysis guarantees the performance of the proposed scheme. In addition, two illustrative examples are presented to validate the efficacy of the proposed scheme and the theoretical results. Moreover, an application to mobile robot navigation in a maze further substantiates the efficacy of the proposed scheme.