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1.
Hydrothermal synthesis using graphene oxide (GO) as a precursor has been used to produce luminescent graphene quantum dots (GQDs). However, such a method usually requires many reagents and multistep pretreatments, while can give rise to GQDs with low quantum yield (QY). Here, we investigated the concentration, the temperature of synthesis, and the pH of the GO solution used in the hydrothermal method through factorial design experiments aiming to optimize the QY of GQDs to reach a better control of their luminescent properties. The best synthesis condition (2 mg/mL, 175 °C, and pH = 8.0) yielded GQDs with a relatively high QY (8.9%) without the need of using laborious steps or dopants. GQDs synthesized under different conditions were characterized to understand the role of each synthesis parameter in the materials' structure and luminescence properties. It was found that the control of the synthesis parameters enables the tailoring of the amount of specific oxygen functionalities onto the surface of the GQDs. By changing the synthesis' conditions, it was possible to prioritize the production of GQDs with more hydroxyl or carboxyl groups, which influence their luminescent properties. The as-developed GQDs with tailored composition were used as luminescent probes to detect Fe3+. The lowest limit of detection (0.136 μM) was achieved using GQDs with higher amounts of carboxylic groups, while wider linear range was obtained by GQDs with superior QY. Thus, our findings contribute to rationally produce GQDs with tailored properties for varied applications by simply adjusting the synthesis conditions and suggest a pathway to understand the mechanism of detection of GQDs-based optical sensors.  相似文献   
2.
针对考虑几何和材料非线性的石英晶体板厚度剪切振动和弯曲振动的方程组,利用扩展伽辽金法对该方程组进行转化和求解,分别获得了强烈耦合的厚度剪切振动模态和弯曲振动模态的频率响应关系,绘制了不同振幅比和不同驱动电压影响下的频率响应曲线图。数值计算结果表明可以选取石英晶片的最佳长厚比尺寸来避免两种模态的强烈耦合。驱动电压的变化将引起石英晶体谐振器厚度剪切振动频率的明显改变,必须将振动频率的漂移值控制在常用压电声波器件的允许值之内。扩展伽辽金法对石英晶体板非线性振动方程组的求解为非线性有限元分析和偏场效应分析奠定了基础。  相似文献   
3.
In the present paper,we study the restricted inexact Newton-type method for solving the generalized equation 0∈f(x)+F(x),where X and Y are Banach spaces,f:X→Y is a Frechet differentiable function and F:X■Y is a set-valued mapping with closed graph.We establish the convergence criteria of the restricted inexact Newton-type method,which guarantees the existence of any sequence generated by this method and show this generated sequence is convergent linearly and quadratically according to the particular assumptions on the Frechet derivative of f.Indeed,we obtain semilocal and local convergence results of restricted inexact Newton-type method for solving the above generalized equation when the Frechet derivative of f is continuous and Lipschitz continuous as well as f+F is metrically regular.An application of this method to variational inequality is given.In addition,a numerical experiment is given which illustrates the theoretical result.  相似文献   
4.
The process of the formation of silver nanoparticles (AgNPs) via the method of galvanic replacement (GR) of Ag+ with aluminum powder in sodium polyacrylate (NaPA) solutions in the ultrasonic (US) field has been studied. It was observed, that the yellow colloidal solutions of stabilized AgNPs with the absorption maximum at ∼ 410 nm were obtained under the application of US power by 20 W and frequency by 20 kHz in the wide range of AgNO3 and NaPA concentrations (0.1 – 0.5 mM and 0.5 – 5.0 g/L respectively) at 25 0C. It was shown, that the GR process under US field occurs without of the significant induction period. Using the UV–vis spectroscopy the kinetics of AgNPs formation has been studied and it was observed the first order kinetics with respect to Ag+ ions both for the nucleation and growth processes. It was found that observable rate constants of nucleation are close for the all experimental conditions but the observable rate constants of growth decreased with increasing of initial concentration of AgNO3. Based on the obtained kinetic data it was proposed a mechanism of the formation of AgNPs consisted of the following two main stages: 1) the nucleation with the formation of primary nanoclusters (AgNCs) on aluminum surface followed by their ablation from the surface of the sacrificial metal by ultrasound into bulk of solution; 2) the transformation of AgNCs in AgNPs via growth from the Al surface and / or agglomeration of AgNCs. Using TEM it was found that the size of obtained AgNPs does not exceed of 25 nm and slightly depends on the initial concentrations of precursors. High antimicrobial activity of obtained colloidal solutions against gram-negative and gram-positive bacteria as well as against fungi was observed.  相似文献   
5.
采用水热-煅烧法制备Cd2SnO4,之后通过超声混合法得到一系列MoS2/Cd2SnO4复合材料。采用X射线衍射、扫描电子显微镜、X射线光电子能谱对Cd2SnO4和一系列MoS2/Cd2SnO4复合材料进行结构和形貌的表征。研究了MoS2掺杂量对于MoS2/Cd2SnO4复合材料的气敏性能影响。实验结果表明,当MoS2与Cd2SnO4的质量比为2.5%,MoS2/Cd2SnO4复合材料制备的气敏元件在170 ℃时对浓度为100 μL·L-1的甲醛气体的灵敏度为40.0,最低检测限为0.1 μL·L-1。  相似文献   
6.
The backbone structure (1,3,4-thiadiazole sulfone derivatives containing amide moiety) of target compounds was determined by modification and optimization of the theoretical design based on commercial chemical carboxin, including molecular docking, scaffold hopping, ligand expansion, etc.In this paper, 23 target compounds were synthesized by the combination of theoretical design and chemical synthesis, and characterized by 1H NMR, 13C NMR and HR MS. Addtionally, the antibacterical bioassay showed that most target compounds performed excellent inhibition on Xanthomonas axonopodis pv. citri (Xac) and Xanthomonas oryzae pv. oryzae (Xoo) in vitro. Meanwhile, molecular docking, molecular dynamics (MD) simulations, and studies on ligand/protein (carboxin/2FBW and 4n/2FBW) complex systems were displayed, and the interaction patterns of ligand/protein complex system were predicted by molecular docking. Besides, the ligand/protein complex system was subject to MD simulation. The analysis of molecular dynamics such as RMSD values suggested that compound/2FBW complexes were stable. MM/GBSA (Molecular mechanics generalized born surface area) dynamic binding affinity results revealed that the active residues (TYR58, HIS26, ARG43, SER39, etc.) played an essential part in the binding of the compound(s) to form a stable low-energy ligand/protein complex, while the MD trajectories demonstrated that the interactions of drugs with 2FBW affected the tertiary structure and increased the stability of protein. Besides, compound 4n also showed control efficacies (curative and protective) on Xoo in vivo, where the curative efficacy was 35.91% and the protective efficacy was 18.97%. In a word, this study showed that 1,3,4-thiadiazole sulfone derivatives containing amide moiety designed based on the structure of carboxin were promising agricultural antibacterial agents, featuring certain stability of binding affinity to proteins and carboxin.  相似文献   
7.
The reaction of N2 with trinuclear niobium and tungsten sulfide clusters Nb3Sn and W3Sn (n=0–3) was systematically studied by density functional theory calculations with TPSS functional and Def2-TZVP basis sets. Dissociations of N−N bonds on these clusters are all thermodynamically allowed but with different reactivity in kinetics. The reactivity of Nb3Sn is generally higher than that of W3Sn. In the favorite reaction pathways, the adsorbed N2 changes the adsorption sites from one metal atom to the bridge site of two metal atoms, then on the hollow site of three metal atoms, and at that place, the N−N bond dissociates. As the number of ligand S atoms increases, the reactivity of Nb3Sn decreases because of the hindering effect of S atoms, while W3S and W3S2 have the highest reactivity among four W3Sn clusters. The Mayer bond order, bond length, vibrational frequency, and electronic charges of the adsorbed N2 are analyzed along the reaction pathways to show the activation process of the N−N bond in reactions. The charge transfer from the clusters to the N2 antibonding orbitals plays an essential role in N−N bond activation, which is more significant in Nb3Sn than in W3Sn, leading to the higher reactivity of Nb3Sn. The reaction mechanisms found in this work may provide important theoretical guidance for the further rational design of related catalytic systems for nitrogen reduction reactions (NRR).  相似文献   
8.
0.5 mol% Nd-doped (Ba0.85Ca0.15)(Ti0.9Hf0.1)O3 (BCTH-Nd) lead-free ceramics were prepared by a solid-phase twin crystal method, where the effects of sintering condition on structure, electrical and optical properties were studied. All the sintered BCTH-Nd ceramics exhibit pure perovskite structure, dense microstructure with several micron grain size, which tends to increase with elevating sintering temperature. All synthesized ceramics have complex dielectric behavior, which presents normal ferroelectrics characteristic with slight dispersion phenomenon. The BCTH-Nd ceramics exhibit excellent piezoelectric and ferroelectric properties and acceptable dielectric performance when sintered at 1480 °C for 2 h. Under 269 nm light excitation, several fluorescent emission peaks are excited with a whole indigo fluorescence, where the strongest emission peak is emitted at 473 nm, corresponding to the 4G3/2 → 4I9/2 energy level transition of Nd3+. Multifunctional performance is fulfilled in the lead-free BCTH ceramics via rare earth doping, which can broaden the application fields of piezoelectric-based materials.  相似文献   
9.
结合无网格局部彼得洛夫-伽辽金(MLPG)方法和径向基函数有限差分(RBF-FD)无网格方法求解非线性热传导问题。MLPG方法属于弱式无网格方法,具有处理边界条件方便的优点,然而因其要做大量的插值、积分运算而计算效率偏低;RBF-FD无网格方法属于强式无网格方法,直接对微分算子进行数值离散,计算效率高,然而其边界条件的处理较复杂。将二者相结合,在求解域边界附近采用MLPG方法,其它区域采用RBF-FD无网格方法,则能扬长避短。介绍了MLPG方法和RBF-FD无网格方法的基本原理,将该混合方法用来求解非线性热传导方程,数值算例显示了方法的正确性和高效性。  相似文献   
10.
沈荣晨  郝磊  陈晴  郑巧清  张鹏  李鑫 《物理化学学报》2022,38(7):2110014-41
随着化石燃料使用的增加和温室气体排放量持续上升,20世纪以来气温上升得更快。开发环境友好型能源取代传统化石燃料是当务之急。氢能源作为一种清洁、高效的能源,被认为是最有希望取代传统化石燃料的能源。光催化水分解水产氢作为为一种环保型技术被认为是最有前景的氢能生产方法。提高光生电子-空穴对分离效率是构建高效光催化剂的关键。然而,利用高度分散的助催化剂构建高效、稳定的产氢光催化剂仍然是一个挑战。本文首次成功地采用一步原位高温磷化法制备了高度分散的非贵金属三金属过度金属磷化Co0.2Ni1.6Fe0.2P助催化剂(PCNS-CoNiFeP)掺杂P的石墨相氮化碳纳米片(PCNS)。有趣的是,PCNS-CoNiFeP与传统氢氧前驱体磷化法制备的CoNiFeP相比,没有聚集性,分散性高。X射线衍射(XRD)、X射线光电子能谱(XPS)、元素映射图像和高分辨率透射电镜(HRTEM)结果表明,PCNS-CoNiFeP已成功合成。紫外-可见吸收光谱结果表明,PCNS-CoNiFeP在200–800 nm波长范围内较PCNS略有增加。光致发光光谱、电化学阻抗谱(EIS)和光电流分析结果表明,CoNiFeP助催化剂能有效促进光生电子-空穴对的分离,加速载流子的迁移。线性扫描伏安法(LSV)结果还表明,负载CoNiFeP助催化剂可大大降低CNS的过电位。结果表明,以三乙醇胺溶液为牺牲剂的PCNS-CoNiFeP最大产氢速率为1200 μmol·h-1·g-1,是纯CNS-Pt (320 μmol·h-1·g-1)的4倍。在420 nm处的表观量子效率为1.4%。PCNS-CoNiFeP在光催化反应中也表现出良好的稳定性。透射电镜结果表明,6–8 nm的CoNiFeP高度分散在PCNS表面。高度分散的CoNiFeP比聚集的CoNiFeP具有更好的电荷分离能力和更高的电催化析氢活性。由此可见,聚合的CoNiFeP-PCNs (300 μmol·h-1·g-1)的产氢速率远低于PCNS-CoNiFeP。此外,CNS的P掺杂可以改善其电导率和电荷传输。  相似文献   
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