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1.
Inorg Chem ; 58(13): 8866-8876, 2019 Jul 01.
Article in English | MEDLINE | ID: mdl-31247873

ABSTRACT

ß-Na2TeO4 is able to trap CO2 in a humid atmosphere due to a partial Na+/H+ exchange and the formation of NaHCO3. The RT powder X-ray diffraction pattern of the resulting Na2- xH xTeO4 shows broad and narrow hkl lines preventing the structural study. We show by the DIFFaX program that Na+/H+ exchange is topotactic since the structure, as in the mother form, consists of [TeO4] n2 n- chains of TeO6 octahedra. We also show that the broadening of some hkl lines is due to stacking faults which result from the weakness of H-O···H bonds connecting the [TeO4] n2 n- chains. Upon heating, a progressive structural organization takes place which has been followed by powder X-ray diffraction, Raman, and NMR spectroscopies. Around 300 °C, a well organized structure can be described from powder X-ray diffraction refinements in the monoclinic P21/ n space group while ab initio computations allowed location of the hydrogen atoms with satisfactory H-O bonds. In addition, we present the CO2 sorption/desorption by Na2TeO4 and compare its performance to that of Na2SiO3. Finally, the existence of a Na2- xLi xTeO4 solid solution (0 ≤ x ≤ 0.9) is evidenced, and we show that the presence of lithium in the structure leads to the disappearance of the structural transition observed for ß-Na2TeO4 and to a progressive decrease of the CO2 capture ability.

2.
Inorg Chem ; 57(12): 7334-7345, 2018 Jun 18.
Article in English | MEDLINE | ID: mdl-29870231

ABSTRACT

The present work concerns the tellurate Na2TeO4 which has a 1D structure and could then present a CO2 capture ability. It has been synthesized in a powder form via a solid-state reaction and structurally characterized by thermal X-ray diffraction experiments, Raman spectroscopy, and differential scanning calorimetry. The room temperature structure corresponds to the ß-Na2TeO4 orthorhombic form, and we show that it undergoes a reversible structural transition near 420 °C toward a monoclinic system. Ab initio computations were also performed on the room temperature structure, the Raman vibration modes calculated, and a normal mode attribution proposed. In agreement with our expectations, this sodium oxide is able to trap CO2 by a two-step mechanism: Na+/H+ exchange and carbonation of the released sodium as NaHCO3. This capture is reversible since CO2 can be released upon heating by recombination of the mother phase.

3.
Dalton Trans ; 43(39): 14841-50, 2014 Oct 21.
Article in English | MEDLINE | ID: mdl-25164264

ABSTRACT

The present work concerns the thermal structural characterization of the acentric Ruddlesden-Popper LiHSrTa2O7. A previous study, performed with powder neutron diffraction data, has revealed that at room temperature, LiHSrTa2O7 crystallizes in the Ama2 space group and that the acentric character is mainly due to the unequal distribution of the Li(+) and H(+) cations on their sites. In this new paper, the thermal behaviour has been studied by several techniques: powder X-ray and neutron diffraction, SHG experiments and Raman spectroscopy. All of them have revealed that LiHSrTa2O7 undergoes a reversible structural transition from an orthorhombic to a tetragonal symmetry around 200 °C. This transition is associated with the progressive vanishing of the TaO6 octahedra tilting, becoming completely straight in the high temperature form (S.G. I4/mmm), and with a variation of the Li(+) and H(+) distribution in the interlayer spacing.

4.
J Phys Chem B ; 113(52): 16465-71, 2009 Dec 31.
Article in English | MEDLINE | ID: mdl-19994880

ABSTRACT

Poly(ethylene oxide) and complexes of lithium trifluorosulfonate-poly(ethylene oxide) (LiTf-PEO) with 4

5.
Langmuir ; 24(19): 11182-8, 2008 Oct 07.
Article in English | MEDLINE | ID: mdl-18729490

ABSTRACT

Amorphous CdSe nanoparticles were prepared by a base-catalyzed room-temperature reaction between cadmium nitrate and selenourea, with dodecanethiol as a capping ligand. The nanoparticle size could be controlled from 1.9 to 3.6 nm by increasing the water concentration in the reaction. When the nanoparticles were heated in a pyridine suspension, excitonic peaks appeared in the initially featureless optical absorption spectra. By changing the suspension solvent and the capping ligand and its concentration, it was shown that the dynamic surface exchange between the ligand and pyridine controls the crystallization process. This phenomenon was interpreted as a surface rigidity effect imposed by the ligand, whose importance was separately evidenced on the dried nanoparticles by the evolution of X-ray diffraction patterns and Raman spectra. In particular, both techniques showed that a threshold temperature is needed before crystallization occurs, and such a threshold was related to ligand desorption. The surface effect was directly visualized by high-resolution transmission electron microscopy observations of the amorphous particles, where crystallization under the electron beam was observed to start by the formation of a crystalline nucleus in the nanoparticle interior and then to extend to the whole structure.

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