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22.
Dmitrii O. Kharchenko Olga M. Shchokotova Vasyl O. Kharchenko Viktor V. Kupriienko S.V. Kokhan Xiaoyong Wu 《辐射效应与固体损伤》2020,175(7-8):602-626
ABSTRACT We study microstructure transformation in Zr–Nb system under neutron irradiation and its mechanical properties change under mechanical loads in a form of shear deformation by using phase field methodology. The developed phase field approach takes into account defects dynamics based on reaction rate theory and elastic contribution to study mechanical properties change. A numerical modeling is provided in three stages: sample preparation, irradiation of the prepared sample and mechanical loading of the irradiated sample. A precipitation of β-Niobium particles of the size of several nanometers is discussed. Results of phase field modeling indicate that β-Niobium particles grow slowly during irradiation due to point defects rearrangement. Statistical analysis of dynamics of radiation-induced microstructure transformations is provided. Simulation results of shear deformation of pre-irradiated and post-irradiated alloys are discussed. Maps of local distribution of strain and stress and strain–stress curves are obtained. Results are verified with experimental data. 相似文献
23.
Dr. Peiyu Ge Dr. Mohamad Hojeij Dr. Micheál D. Scanlon Prof. Hubert H. Girault 《Chemphyschem》2020,21(24):2630-2633
H2 may be evolved biphasically using a polarised liquid|liquid interface, acting as a “proton pump”, in combination with organic soluble metallocenes as electron donors. Sustainable H2 production requires methodologies to recycle the oxidised donor. Herein, the photo-recycling of decamethylferrocenium cations (DcMFc+) using aqueous core-shell semiconductor CdSe@CdS nanoparticles is presented. Negative polarisation of the liquid|liquid interface is required to extract DcMFc+ to the aqueous phase. This facilitates the efficient capture of electrons by DcMFc+ on the surface of the photo-excited CdSe@CdS nanoparticles, with hydrophobic DcMFc subsequently partitioning back to the organic phase and resetting the system. TiO2 (P25) and CdSe semiconductor nanoparticles failed to recycle DcMFc+ due to their lower conduction band energy levels. During photo-recycling, CdS (on CdSe) may be self-oxidised and photo-corrode, instead of water acting as the hole scavenger. 相似文献
24.
本文采用关联分析方法研究了稳定温度分层湍流中的结构特性、输运特性,以及热量、动量逆梯度输运现象的尺度效应及其参数演化.首先采用大涡模拟方法对稳定分层湍流中的结构特性和输运特性进行了分析,将逆梯度输运发生的时间尺度作为已知条件,结合关联量分析方法在波数空间中的解析解,对逆梯度输运现象的尺度效应进行了分析研究.结果发现,稳定分层强度较大的流动中发生垂向热量及动量逆梯度输运现象,发生的结构尺度与关联分析所发现垂向热量、动量逆梯度输运的波数形成了呼应.随着分层强度增加,热量、动量的输运强度均受抑制,与逆梯度输运关联的流场结构尺度减小,同样的效应也发生在流场结构向下游演化的过程中. 相似文献
25.
Xu Liu Ruoyu Liu Jiaxing Qiu Prof. Dr. Xu Cheng Prof. Dr. Guigen Li 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(33):14066-14071
We report a method for the electrochemical deuteration of α,β-unsaturated carbonyl compounds under catalyst- and external-reductant-free conditions, with deuteration rates as high as 99 % and yields up to 91 % in 2 h. The use of graphite felt for both the cathode and the anode was key to ensuring chemoselectivity and high deuterium incorporation under neutral conditions without the need for an external reductant. This method has a number of advantages over previously reported deuteration reactions that use stoichiometric metallic reductants. Mechanistic experiments showed that O2 evolution at the anode not only eliminates the need for an external reductant but also regulates the pH of the reaction mixture, keeping it approximately neutral. 相似文献
26.
Dr. Hui Chen Lei Shi Xiao Liang Lina Wang Prof. Tewodros Asefa Prof. Xiaoxin Zou 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(44):19822-19826
Reducing the amount of iridium in oxygen evolution electrocatalysts without compromising their catalytic performances is one of the major requirements in proton-exchange-membrane water electrolyzers. Herein, with the help of theoretical studies, we show that anatase-type TiO2-IrO2 solid solutions possess more active iridium catalytic sites for the oxygen evolution reaction (OER) than IrO2, the benchmark OER catalyst. Note that the same is not observed for their rutile-type counterparts. However, owing to their thermodynamic metastability, anatase-type TiO2-IrO2 solid solutions are generally hard to synthesize. Our theoretical studies demonstrate that such catalytically active anatase-type solid-solution phases can be created in situ on the surfaces of readily available SrTiO3-SrIrO3 solid solutions during electrocatalysis in acidic solution as the solution can etch away Sr atoms. We experimentally show this with porous SrTiO3-SrIrO3 solid-solution nanotubes synthesized by a facile synthetic route that contain 56 % less iridium than IrO2 yet show an order of magnitude higher apparent catalytic activity for OER in acidic solution. 相似文献
27.
Dr. Yong-Sheng Wei Dr. Liming Sun Miao Wang Dr. Jinhua Hong Dr. Lianli Zou Hongwen Liu Dr. Yu Wang Dr. Mei Zhang Dr. Zheng Liu Prof. Yinwei Li Prof. Satoshi Horike Prof. Kazu Suenaga Prof. Qiang Xu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(37):16147-16156
Understanding the thermal aggregation behavior of metal atoms is important for the synthesis of supported metal clusters. Here, derived from a metal–organic framework encapsulating a trinuclear FeIII2FeII complex (denoted as Fe3) within the channels, a well-defined nitrogen-doped carbon layer is fabricated as an ideal support for stabilizing the generated iron nanoclusters. Atomic replacement of FeII by other metal(II) ions (e.g., ZnII/CoII) via synthesizing isostructural trinuclear-complex precursors (Fe2Zn/Fe2Co), namely the “heteroatom modulator approach”, is inhibiting the aggregation of Fe atoms toward nanoclusters with formation of a stable iron dimer in an optimal metal–nitrogen moiety, clearly identified by direct transmission electron microscopy and X-ray absorption fine structure analysis. The supported iron dimer, serving as cooperative metal–metal site, acts as efficient oxygen evolution catalyst. Our findings offer an atomic insight to guide the future design of ultrasmall metal clusters bearing outstanding catalytic capabilities. 相似文献
28.
Dong-Liang Zhang Cheng-Long Deng Bin Xie Yu-Long Li Chuan Lai Wen-Yu Mou Lin-Xin He Xiao-Xue Bai Tao Li Jia-Xi Cao Jun Wang 《应用有机金属化学》2020,34(1):e5261
Six new O-alkyldithiophosphate nickel complexes with dcpf ligand, [(dcpf)Ni(S2P{O}OR)] (dcpf = 1,1′-bis (dicyclohexylphosphino)ferrocene, R = CH3 ( 1 ), CH3CH2 ( 2 ), Ph ( 3 ), 4-MeC6H4 ( 4 ), PhCH2 ( 5 ) and PhCH2CH2 ( 6 )), have been synthesized by the treatment of dcpf with ((RO)2PS2)2Ni in satisfactory yields. These complexes were characterized by elemental analysis, spectroscopy (FTIR, UV–vis, 1H, 13C, and 31P NMR), thermogravimetric analysis and single crystal X-ray diffraction. The nickel atom in 1 , 2 ·CH2Cl2, 3 ·CH2Cl2, 4 ·2CH2Cl2·THF, and 2( 5 )·hexane adopts a slightly distorted square-planar coordination environment finished by two phosphorus atoms of dcpf ligand and two sulfur atoms of O-alkyldithiophosphate ligand. Furthermore, the electrochemical properties for complexes 1 – 6 were also investigated by cyclic voltammetry. With the addition of 120 mM trifluoroacetic acid (TFA), the turnover frequency (TOF) values for 1 – 6 are estimated to be 1243.83, 1046.54, 1331.71, 2545.29, 1899.03, and 1191.37 s−1, with the overpotential (η) values of 0.62, 0.58, 0.71, 0.67, 0.60, and 0.56 V, respectively. The result of electrochemical studies indicates that all complexes can be used as efficient molecular eletrocatalysts for the reduction of protons to hydrogen in the presence of TFA in MeCN. 相似文献
29.
Saulius Kaciulis Alessio Mezzi Roberto Montanari Maria Richetta Ekaterina Pakhomova Alessandra Varone 《Surface and interface analysis : SIA》2020,52(12):1093-1097
The W-1%La2O3 alloy has been irradiated by a single laser pulse (λ = 1064 nm) to simulate transient thermal loads of high energy occurring in a tokamak under operative conditions. A zone with a diameter of ~2 mm, namely, much larger than the focal spot, results to be affected by the pulse, and a crater of about 300 μm is observed in its center. La2O3 particles are not present inside the crater. The change of surface morphology is accompanied by elemental redistribution. Multipoint XPS analysis evidenced that the concentration of La is very low in the crater and increases moving toward the border of the affected zone while that of W shows an opposite trend. The composition changes involve only the outmost 5 nm of the sample: through depth profiling, no differences of chemical composition were detected deeper in the alloy between the center and external border of the affected area. 相似文献
30.
Dr. Qi Hu Guomin Li Zhen Han Ziyu Wang Xiaowan Huang Dr. Hengpan Yang Prof. Qianling Zhang Prof. Jianhong Liu Prof. Chuanxin He 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(18):3930-3942
Recently, nonmetal doping has exhibited its great potential for boosting the hydrogen evolution reaction (HER) of transition-metal (TM)-based electrocatalysts. To this end, this work overviews the recent achievements made on the design and development of the nonmetal-doped TM-based electrocatalysts and their performance for the HER. It is also shown that by rationally doping nonmetal elements, the electronic structures of TM-based electrocatalysts can be effectively tuned and in turn the Gibbs free energy of the TM for adsorption of H* intermediates (ΔGH*) optimized, consequently enhancing the intrinsic activity of TM-based electrocatalysts. Notably, we highlight that concurrently doping two nonmetal elements can continuously and precisely regulate the electronic structures of the TM, thereby maximizing the activity for HER. Moreover, nonmetal doping also accounts for enhancing the physical properties of the TM (i.e. surface area). Therefore, nonmetal doping is a robust strategy for simultaneous regulation of the chemical and physical features of the TM. 相似文献