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91.
Alexander A. Kamnev Roman L. Dykman Krisztina Kovács Alexei N. Pankratov Anna V. Tugarova Zoltán Homonnay Ernő Kuzmann 《Structural chemistry》2014,25(2):649-657
Iron(III)-containing aqueous solutions of 5-methylresorcinol (5-MR), 5-n-propylresorcinol (5-n-PR) and 4-n-hexylresorcinol (4-n-HR) at pH ~ 3 were studied by means of 57Fe transmission Mössbauer spectroscopy. Kinetic considerations were applied to the redox reactions. Density Functional Theory (DFT) calculations were performed for the alkylresorcinol (AR) molecules and their non-alkylated analogue (resorcinol). Mössbauer spectra consisted of quadrupole doublets assigned to high-spin Fe(III) and Fe(II) species. From changes in their relative spectral areas, a gradual reduction of Fe(III) by all the ARs studied was observed. However, significant differences were found for the reduction rates among the ARs. The following series of the reduction rates was established by means of Mössbauer spectroscopy: 4-n-HR ? 5-MR > 5-n-PR, supplemented by rate constants calculated using a kinetic model. DFT calculations resulted in the following series: 4-n-HR ? 5-n-PR > 5-MR ? resorcinol (the latter is not oxidised under the conditions applied). The reversed order of the experimentally observed 5-MR and 5-n-PR oxidation rates may be explained in terms of their different kinetic parameters related to their structure. 相似文献
92.
Single‐Crystal‐like Nanoporous Spinel Oxides: A Strategy for Synthesis of Nanoporous Metal Oxides Utilizing Metal‐Cyanide Hybrid Coordination Polymers 下载免费PDF全文
Masataka Imura Rahul R. Salunkhe Naoto Umezawa Hicham Hamoudi Alexei A. Belik Yusuke Yamauchi 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(52):17375-17384
Development of a new method to synthesize nanoporous metal oxides with highly crystallized frameworks is of great interest because of their wide use in practical applications. Here we demonstrate a thermal decomposition of metal‐cyanide hybrid coordination polymers (CPs) to prepare nanoporous metal oxides. During the thermal treatment, the organic units (carbon and nitrogen) are completely removed, and only metal contents are retained to prepare nanoporous metal oxides. The original nanocube shapes are well‐retained even after the thermal treatment. When both Fe and Co atoms are contained in the precursors, nanoporous Fe?Co oxide with a highly oriented crystalline framework is obtained. On the other hand, when nanoporous Co oxide and Fe oxide are obtained from Co‐ and Fe‐contacting precursors, their frameworks are amorphous and/or poorly crystallized. Single‐crystal‐like nanoporous Fe?Co oxide shows a stable magnetic property at room temperature compared to poly‐crystalline metal oxides. We further extend this concept to prepare nanoporous metal oxides with hollow interiors. Core‐shell heterostructures consisting of different metal‐cyanide hybrid CPs are prepared first. Then the cores are dissolved by chemical etching using a hydrochloric acid solution (i.e., the cores are used as sacrificial templates), leading to the formation of hollow interiors in the nanocubes. These hollow nanocubes are also successfully converted to nanoporous metal oxides with hollow interiors by thermal treatment. The present approach is entirely different from the surfactant‐templating approaches that traditionally have been utilized for the preparation of mesoporous metal oxides. We believe the present work proves a new way to synthesize nanoporous metal oxides with controlled crystalline frameworks and architectures. 相似文献
93.
Jagodige P. Yasomanee Prof. Alexei V. Demchenko 《Angewandte Chemie (International ed. in English)》2014,53(39):10453-10456
A Hydrogen bond mediated aglycone delivery (HAD) method was applied to the synthesis of α‐glucans, which are abundant in nature, but as targets represent a notable challenge to chemists. The synthesis of linear oligosaccharide sequences was accomplished in complete stereoselectivity in all glycosylations. The efficacy of HAD may diminish with the increased bulk of the glycosyl acceptor, and may be an important factor for the syntheses of oligomers beyond pentasaccharides. The synthesis of a branched structure proved more challenging, particularly with bulky trisaccharide acceptors. 相似文献
94.
Pressure-induced insulator-to-metal transition (IMT) has been studied in the van der Waals compound iron thiophosphate (FePS3) using first-principles calculations within the periodic linear combination of atomic orbitals method with hybrid Hartree–Fock-DFT B3LYP functional. Our calculations reproduce correctly the IMT at ∼15 GPa, which is accompanied by a reduction of the unit cell volume and of the vdW gap. We found from the detailed analysis of the projected density of states that the 3p states of phosphorus atoms contribute significantly at the bottom of the conduction band. As a result, the collapse of the band gap occurs due to changes in the electronic structure of FePS3 induced by relative displacements of phosphorus or sulfur atoms along the c-axis direction under pressure. 相似文献
95.
Tao Zhang Jingxiang Low Jiaguo Yu Alexei M. Tyryshkin Elika Mikmekov Tewodros Asefa 《Angewandte Chemie (International ed. in English)》2020,59(35):15000-15007
A mesoporous TiO2?x material comprised of small, crystalline, vacancy‐rich anatase nanoparticles (NPs) shows unique optical, thermal, and electronic properties. It is synthesized using polymer‐derived mesoporous carbon (PDMC) as a template. The PDMC pores serve as physical barriers during the condensation and pyrolysis of a titania precursor, preventing the titania NPs from growing beyond 10 nm in size. Unlike most titania nanomaterials, during pyrolysis the NPs undergo no transition from the anatase to rutile phase and they become catalytically active reduced TiO2?x. When exposed to a slow electron beam, the NPs exhibit a charge/discharge behavior, lighting up and fading away for an average period of 15 s for an extended period of time. The NPs also show a 50 nm red‐shift in their UV/Vis absorption and long‐lived charge carriers (electrons and holes) at room temperature in the dark, even long after UV irradiation. The NPs as photocatalysts show a good activity for CO2 reduction. 相似文献
96.
V. A. Dergachev S. S. Vasiliev O. M. Raspopov H. Jungner 《Bulletin of the Russian Academy of Sciences: Physics》2011,75(6):847-850
The possible influence of changes in cosmic ray fluxes on climate variability has been the subject of wide speculation in
recent years. New studies show that the interrelation between the parameters of the geomagnetic field and climate can also
be followed on time scales of different lengths. We present our analysis of data on cosmic rays and changes in climate and
the geomagnetic field obtained from different natural archives. 相似文献
97.
Classical molecular dynamics simulations have been performed for crystalline germanium with the aim to estimate the thermal
effects within the first three coordination shells and their influence on the single-scattering and multiple-scattering contributions
to the Ge K-edge extended x-ray absorption fine structure (EXAFS). 相似文献
98.
Alexei Borodin Mihail Poplavskyi Christopher D. Sinclair Roger Tribe Oleg Zaboronski 《Communications in Mathematical Physics》2016,346(3):1051-1055
We correct an error in Theorem 12 of the original article concerning the edge scaling limit of the law of real eigenvalues for the real Ginibre ensemble. 相似文献
99.
100.
Let be an oriented Jordan smooth curve and a diffeomorphism of onto itself which has an arbitrary nonempty set of periodic points. We prove criteria for one-sided invertibility of the binomial functional operator
wherea andb are continuous functions,I is the identity operator,W is the shift operator,Wf=fo, on a reflexive rearrangement-invariant spaceX() with Boyd indices
X
,
X
and Zippin indicesp
x,q
x satisfying inequalities
Partially supported by F.C.T. (Portugal) grant PRAXIS XXI/BPD/22006/99.Partially supported by CONCACYT (México) grant, Cátedra Patrimonial, No. 990017-EX., nivel II. 相似文献