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1.
Employing nanocrystals (NCs) as building blocks of porous aerogel network structures allows the conversion of NC materials into macroscopic solid structures while conserving their unique nanoscopic properties. Understanding the interplay of the network formation and its influence on these properties like size-dependent emission is a key to apply techniques for the fabrication of novel nanocrystal aerogels. In this work, CdSe/CdS dot/rod NCs possessing two different CdSe core sizes were synthesized and converted into porous aerogel network structures. Temperature-dependent steady-state and time-resolved photoluminescence measurements were performed to expand the understanding of the optical and electronic properties of these network structures generated from these two different building blocks and correlate their optical with the structural properties. These investigations reveal the influence of network formation and aerogel production on the network-forming nanocrystals. Based on the two investigated NC building blocks and their aerogel networks, mixed network structures with various ratios of the two building blocks were produced and likewise optically characterized. Since the different building blocks show diverse optical response, this technique presents a straightforward way to color-tune the resulting networks simply by choosing the building block ratio in connection with their quantum yield.  相似文献   
2.
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   
3.
A magnetically separable palladium nanocatalyst has been synthesized through the immobilization of palladium onto 3-aminopropylphenanthroline Schiff based functionalized silica coated superparamagnetic Fe3O4 nanoparticles. The nanocatalyst (Fe3O4@SiNSB-Pd) was fully characterized using several spectroscopic techniques, such as FT-IR, HR-SEM, TEM, XRD, ICP, and XPS. The microscopic image of Fe3O4 showed spherical shape morphology and had an average size of 150 nm. The Pd-nanoparticles exhibited an average size 3.5 ± 0.6 nm. The successful functionalization of Fe3O4@SiNSB-Pd was identified by FT-IR spectroscopy and the appearance of palladium species in Fe3O4@SiNSB-Pd was confirmed by XRD analysis. While XPS has been utilized for the determination of the chemical oxidation state of palladium species in Fe3O4@SiNSB-Pd. Several activated and deactivated arene halides and olefines were employed for Mizoroki-Heck cross-coupling reactions in the presence of Fe3O4@SiNSB-Pd, each of which produced the respective cross-coupling products with excellent yields. The Fe3O4@SiNSB-Pd shows good reactivity and reusability for up to seven consecutive cycles.  相似文献   
4.
660 MW超临界W火焰锅炉低负荷稳燃特性研究   总被引:1,自引:0,他引:1  
“碳中和”、“碳达峰”的提出预示着未来煤电机组将在更低的负荷运行,用于燃烧无烟煤、贫煤等低挥发份煤种的W火焰锅炉低负荷运行时会出现燃烧稳定性问题。以某660 MW超临界W型火焰锅炉为对象开展了针对低负荷稳燃特性的研究,进行了100%、60%、55%、45%THA工况的试验研究与数值模拟解析,35%THA工况理论预报。结果表明由于炉膛温度降低、煤粉变细、煤粉浓度降低的综合影响,负荷对煤粉颗粒的着火距离影响不大;低负荷工况下投运两侧燃烧器、减少乏气风的射入量有利于提高燃烧稳定性;通过数值模拟可知35%THA工况无法保持炉内高温火焰稳定燃烧,模拟预报锅炉会熄火。  相似文献   
5.
We study the local stability near the maximum figure of merit for the low-dissipation cyclic refrigerator,where the irreversible dissipation occurs not only in the thermal contacts but also the adiabatic strokes.We find that the bounds of the coefficient of performance at a maximum figure of merit or maximum cooling rate in the presence of internal dissipation are identical to those in the corresponding absence of internal dissipation.Using two different scenarios,we prove the existence of a single stable steady state for the refrigerator,and clarify the role of internal dissipation on the stability of the thermodynamic steady state,showing that the speed of system evolution to the steady state decreases due to internal dissipation.  相似文献   
6.
DNA methyltransferase (DNA MTase) can act as biomarker for many diseases and it is important to develop some new methods for sensitive detection of DNA MTase. In this work, a highly efficient electrochemiluminescence (ECL) sensor had been designed for detection of DNA MTase based on Ru(phen)32+ loaded double strand DNA (dsDNA- Ru(phen)32+) as signal tags. Ru(phen)32+ had been efficiently embed in the dsDNA produced through a simple hybridization chain reaction. First, a hairpin probe was designed, which can be specifically recognized by Dam MTase and modified with -SH at one end. It was modified on the surface of gold electrode by -SH as an immobilization probe (IP). This IP will be methylated in the present of Dam MTase and digested by DpnI following. Results in the release of capture probe (CP) which remains on the surface of gold electrode. The CP can hybridize with the single stand part of the dsDNA- Ru(phen)32+ and make the immobilization of ECL tags on the electrode surface, which results in a strong ECL signals detected. However, without the effect of Dam MTase, the hairpin structure of IP remains stable and cannot capture signal tags, and can only detecte weak ECL signals. The biosensor can detect the activity of Dam MTase in the concentration range of 0.01 U/mL to 20 U/mL with the ECL intensity and the logarithm of the concentration have a linear relationship, and the detection limit is calculated to be 7.6 mU/mL. The developed sensor has the ability to specifically detect Dam MTase, which can be differentiated from other types of DNA MTase. In addition, the designed method has good applicability to detect Dam MTase activity in serum samples and been applied to detect its inhibitor with high efficiency.  相似文献   
7.
Lijun Ni 《中国物理 B》2022,31(12):128504-128504
We report the temperature dependence of the spin pumping effect for Y3Fe5O12 (YIG, 0.9 μm)/NiO (tNiO)/W (6 nm) (tNiO = 0 nm, 1 nm, 2 nm, and 10 nm) heterostructures. All samples exhibit a strong temperature-dependent inverse spin Hall effect (ISHE) signal Ic and sensitivity to the NiO layer thickness. We observe a dramatic decrease of Ic with inserting thin NiO layer between YIG and W layers indicating that the inserting of NiO layer significantly suppresses the spin transport from YIG to W. In contrast to the noticeable enhancement in YIG/NiO (tNiO ≈ 1-2 nm)/Pt, the suppression of spin transport may be closely related to the specific interface-dependent spin scattering, spin memory loss, and spin conductance at the NiO/W interface. Besides, the Ic of YIG/NiO/W exhibits a maximum near the TN of the AF NiO layer because the spins are transported dominantly by incoherent thermal magnons.  相似文献   
8.
The requirement of green and sustainable materials to prepare heterogeneous catalysts has intensified for practical reasons over the past few decades. Carbohydrates are possibly the most plentiful and renewable organic materials in nature with inimitable physiochemical properties, plausible low-cost and large-scale production, and sustainability features could be exploited in the generation of nanostructured heterogeneous catalysts. This review article outlines the organic transformations catalyzed by diverse carbohydrate-based nanostructured catalysts in greener and environmentally friendly processes. Selected examples are highlighted for a variety of organic reactions exploiting the proposed catalysts’ reactivity and reusability, and interactions with the intrinsic nature of the applied carbohydrate supports; advantages and speculated challenges of the introduced catalysts are deliberated as well.  相似文献   
9.
本文设计了一种梯形的周期极化掺镁铌酸锂(PPMgLN)波导,并通过在传播方向上引入温度梯度来拓宽其倍频(SHG)过程的泵浦光源可接收带宽。通过有限差分的光束传输法,计算波导的有效折射率,并进行波导尺寸的设计。结果表明,通过改变梯形波导不同位置的温度,使其形成一个温度梯度,可拓宽泵浦光源的波长可接收带宽。本文所设计的PPMgLN波导最大泵浦光源可接收带宽为C波段,即1 530~1 565 nm,该波导可倍频C波段,得到输出波段带宽为765~782.5 nm,温度调谐范围为30~150 ℃。  相似文献   
10.
Zhengran Wang 《中国物理 B》2022,31(4):48202-048202
Excited-state double proton transfer (ESDPT) in the 1-[(2-hydroxy-3-methoxy-benzylidene)-hydrazonomethyl]-naphthalen-2-ol (HYDRAVH2) ligand was studied by the density functional theory and time-dependent density functional theory method. The analysis of frontier molecular orbitals, infrared spectra, and non-covalent interactions have cross-validated that the asymmetric structure has an influence on the proton transfer, which makes the proton transfer ability of the two hydrogen protons different. The potential energy surfaces in both S0 and S1 states were scanned with varying O-H bond lengths. The results of potential energy surface analysis adequately proved that the HYDRAVH2 can undergo the ESDPT process in the S1 state and the double proton transfer process is a stepwise proton transfer mechanism. Our work can pave the way towards the design and synthesis of new molecules.  相似文献   
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