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1.
ACS Omega ; 6(28): 17923-17930, 2021 Jul 20.
Article in English | MEDLINE | ID: mdl-34308027

ABSTRACT

Extracting cesium (Cs) from nonexpandable illite clay is important in the remediation of radioactive Cs-contaminated soil. In this study, we investigated a chloride salt treatment technique for the removal of Cs from illite. Cs-loaded illite samples with initial Cs concentrations of 2430 and 690 ppm were treated using a NaCl-MgCl2-CaCl2 ternary salt system at 400-850 °C under ambient pressure to suppress Cs loss by vaporization. As a result of the treatment at 850 °C, wherein the salt was in a molten state, the Cs concentration was reduced by 99.5% (to 11.6 ppm) in the first sample and by 99.4% (to 3.86 ppm) in the second sample. Cs removal was achieved for these two samples even in a solid-state reaction at 400 °C, with reductions of 83.3% (407 ppm) and 73.3% (184 ppm), respectively. CsCl was formed by the reaction and remained stable in the salt. The incorporation of cations from the salt (mainly Mg2+) to illite induced structural evolution forming an indialite phase to expel Cs from the clay samples.

2.
J Nanosci Nanotechnol ; 16(5): 4516-22, 2016 May.
Article in English | MEDLINE | ID: mdl-27483784

ABSTRACT

PtSn/C and Pt5Sn4M/C (M = W, Pd, Ni) electrocatalysts were prepared by impregnation method using NaBH4 as a reducing agent. Chemical composition, crystalline size, and alloy formation were determined by EDX, XRD and TEM. The average particle sizes of the synthesized catalysts were approximately 3.64-4.95 nm. The electro-chemical properties were measured by CO stripping, cyclic voltammetry, linear sweep voltammetry, and chronoamperometry. The maximum specific activity of the electro-catalysts for ethanol electro-oxidation was 406.08 mA m(-2) in Pt5Sn4Pd/C. The poisoning rate of the Pt5Sn4Pd/C (0.0017% s(-1)) was 4.5 times lower than that of the PtSn/C (0.0076% s(-1)).

3.
J Nanosci Nanotechnol ; 11(1): 810-4, 2011 Jan.
Article in English | MEDLINE | ID: mdl-21446551

ABSTRACT

Both structural refinement using X-ray powder diffraction data and energy calculation using quantum mechanics were used to determine the site preference and the amount of Gd in the host lattice of Gd doped Fe3O4 [Gd(x)Fe(3-x)O4 (x = 0.1)] nanopowder prepared by the sonochemical method. Among possible cation-disorder models, the model proposed by structural refinement, in which Gd ions might preferentially occupy the octahedral sites in Gd doped Fe3O4 having the inverse spinel structure, was confirmed by geometry energy calculation using a first-principle based on the density-functional theory. The final converged weighted R-factor, R(wp), and the goodness-of-fit indicator, S (= R(wp)/R(e)) were 6.73% and 1.22, respectively. The occupancy of Gd ions occupying octahedral sites was 0.04(2).

4.
Phys Chem Chem Phys ; 12(46): 15259-64, 2010 Dec 14.
Article in English | MEDLINE | ID: mdl-20944853

ABSTRACT

A combinatorial library of membrane-electrode-assemblies (MEAs) which consisted of 27 different compositions was fabricated to optimize the multilayer structure of direct methanol fuel cells. Each spot consisted of three layers of ink and a gradient was generated by employing different concentrations of the three components (Pt catalyst, Nafion® and polytetrafluoroethylene (PTFE)) of each layer. For quick evaluation of the library, a high-throughput optical screening technique was employed for methanol electro-oxidation reaction (MOR) activity. The screening results revealed that gradient layers could lead to higher MOR activity than uniform layers. It was found that the MOR activity was higher when the concentrations of Pt catalyst and Nafion ionomer decreased downward from the top layer to the bottom layer. On the other hand, higher MOR activity was observed when PTFE concentration increased downward from the top to the bottom layer.

5.
Langmuir ; 26(21): 16529-33, 2010 Nov 02.
Article in English | MEDLINE | ID: mdl-20504037

ABSTRACT

One of the major issues in direct methanol fuel cell research is to develop a new catalyst for methanol electro-oxidation reaction (MOR) with high activity and low cost. In this study, a new, simple, and economic way was introduced to improve the catalytic activity of commercial PtRu black catalyst for the MOR. A nanocomposite electrode was fabricated by mixing the PtRu catalyst with Fe(2)O(3) nanoclusters. When 10 wt % of the PtRu catalyst was replaced by the Fe(2)O(3) nanoclusters, mass activity (A/g(Pt)) increased by 80% compared to that of the pure PtRu catalyst. Specific activity of the mixed catalyst was 100% higher than that of the pure PtRu catalyst. The nanocomposite catalysts were also applied to single cells. Although the amount of the PtRu catalyst was reduced by 10 wt %, 10% higher potential was observed in the nanocomposite catalysts at a current density of 100 mA/cm(2).


Subject(s)
Alloys/chemistry , Ferrosoferric Oxide/chemistry , Methanol/chemistry , Nanostructures/chemistry , Platinum/chemistry , Ruthenium/chemistry , Catalysis , Electrodes , Electrons , Oxidation-Reduction , Particle Size , Surface Properties
6.
J Comb Chem ; 9(5): 823-7, 2007.
Article in English | MEDLINE | ID: mdl-17665961

ABSTRACT

A ferroelectric Bi4-xLaxTi3O12 (BLT) thin film library was fabricated from Bi2O3/La2O3/TiO2 multilayers using a multitarget RF-sputtering system equipped with an automated shutter. The polarization-electric field and structure were mapped as a function of the La content from x=0 to 1. Remnant polarization (Pr) increased as the La content decreased, and it reached a maximum 2Pr of 20 microC/cm2 at x=0.28. At x<0.28, 2Pr decreased gradually as the La content decreased. This compositional dependence of the remanent polarization was the result of the degree of TiO6 tilting along the a-b plane changing as a function of the La content. This was quantitatively related to the intensity ratio between the (117) peak and the (008) peak in the X-ray diffraction (XRD) pattern and to the intensity of the Raman band at 848 cm-1, arising from stretching mode of TiO6 octahedrons.


Subject(s)
Combinatorial Chemistry Techniques , Spectrum Analysis, Raman/methods , Titanium/chemistry , X-Ray Diffraction/methods , Quantitative Structure-Activity Relationship
7.
Proc Natl Acad Sci U S A ; 104(4): 1134-9, 2007 Jan 23.
Article in English | MEDLINE | ID: mdl-17218453

ABSTRACT

Combinatorial approach for discovering novel functional materials in the huge diversity of chemical composition and processing conditions has become more important for breakthrough in thin film electronic and energy-conversion devices. The efficiency of combinatorial method depends on the preparation of a reliable high-density composition thin-film library. The physico-chemical properties of each sample on the library should be similar to those of the corresponding samples prepared by one-by-one conventional methods. We successfully developed the combinatorial liquid source misted chemical deposition (LSMCD) method and demonstrated its validity in screening the chemical composition of Bi3.75LaxCe0.25-xTi3O12 (BLCT) for high remanent polarization (Pr). LSMCD is a cheap promising combinatorial screening tool. It can control the composition up to ppm level and produce homogeneous multicomponent library. LSMCD method allows us to prepare BLCT thin-film library at the variation of 0.4 mol% of La. Maximum 2Pr is 35 microC/cm-2 at x=0.21. The intensity of (117) XRD peak is quantitatively related to 2Pr. Newly developed scanning piezoelectric deformation measurement for nano-sized samples using scanning probe microscope (SPM) is also found out to be reliable for determining the relative ranking of Pr value rapidly.

8.
J Phys Chem B ; 109(2): 968-72, 2005 Jan 20.
Article in English | MEDLINE | ID: mdl-16866466

ABSTRACT

A combined structural refinement of Bi3.5La0.5Ti3O12 against both neutron and X-ray diffraction data was performed at 298 K on the basis of the Raman study. The upshift of Raman peaks suggested that the substitution sites of La atoms in Bi3.5La0.5Ti3O12 were only the Bi sites in the perovskite units. Of the two crystal structural models (orthorhombic and monoclinic systems) considered for the crystal structural system of Bi3.5La0.5Ti3O12, the weighted R factor, Rwp, and goodness-of-fit indicator, S (=Rwp/Re), of the monoclinic system were lower than those of the orthorhombic one. The final Rwp and S values based on the monoclinic system were 7.04% (6.34 and 7.76% for the neutron data and the X-ray data, respectively) and 1.45, respectively. The lattice parameters obtained from the combined structural refinement were a = 5.4321(1) A, b = 5.4161(1) A, and c = 32.8614(3) A. The beta angle was 89.95(4) degrees . Spontaneous polarizations calculated from the refined structural parameters were 27.0 microC/cm2 for the monoclinic system and 1.8 microC/cm2 for the orthorhombic one.

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