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1.
J Am Chem Soc ; 132(19): 6686-95, 2010 May 19.
Artículo en Inglés | MEDLINE | ID: mdl-20423085

RESUMEN

The energy efficiency of heat engines could be improved by the partial recovery of waste heat using thermoelectric (TE) generators. We show the possibility of designing nanostructured TE materials using colloidal inorganic nanocrystals functionalized with molecular antimony telluride complexes belonging to the family of Zintl ions. The unique advantage of using Zintl ions as the nanocrystal surface ligands is the possibility to convert them into crystalline metal chalcogenides, thus linking individual nanobuilding blocks into a macroscopic assembly of electronically coupled functional modules. This approach allows preserving the benefits of nanostructuring and quantum confinement while enabling facile charge transport through the interparticle boundaries. A developed methodology was applied for solution-based fabrication of nanostructured n- and p-type Bi(2-x)Sb(x)Te(3) alloys with tunable composition and PbTe-Sb(2)Te(3) nanocomposites with controlled grain size. Characterization of the TE properties of these materials showed that their Seebeck coefficients, electrical and thermal conductivities, and ZT values compared favorably with those of previously reported solution-processed TE materials.

2.
J Am Chem Soc ; 128(9): 2931-9, 2006 Mar 08.
Artículo en Inglés | MEDLINE | ID: mdl-16506772

RESUMEN

Mn ion doping of CdSe and other semimagnetic quantum dot (QDs) alloys has been an area of active speculation for over a decade. We report evidence of Mn(II) doping of CdSe grown from a cubic single source precursor that is superparamagnetic (SPM) with a blocking temperature of 40 K following thermal annealing. Prior to thermal annealing the 4 nm Mn/CdSe (1% Mn) QDs exhibit mainly paramagnetic behavior between 300 and 2 K, with a weak antiferromagnetic exchange. Following thermal annealing of the sample, high-temperature ferromagnetic exchange is observed in the magnetization data with the onset of an SPM phase at 40 K that exhibits a coercivity of 0.1 T at 2 K. The switching-on of SPM behavior is believed to be linked to ion migration with formation of (Se-Mn-Se-Mn-Se-Mn)n centers within the nanocrystal that exhibit coupled magnetic moments. Electron paramagnetic resonance (EPR) provides evidence of two distorted T(d) Mn core sites, a clustered site (dipolar broadened), and a localized Mn site (hyperfine-split). The ratio of the EPR signature for the dipolar broadened site increases following annealing and shows a hysteretic response around the blocking temperature. These observations suggest that thermal annealing results in enhanced cluster formation explaining the onset of the SPM phase in these nanoscale materials. Evidence of SPM behavior is evident in the field-dependent non-Langevin magnetization with a tangential loss in the ac-magnetic susceptibility and the Mydosh parameter (phi = 0.16).

3.
Chemistry ; 10(14): 3364-71, 2004 Jul 19.
Artículo en Inglés | MEDLINE | ID: mdl-15252782

RESUMEN

Nanoparticulate transition-metal phosphides remain an unexplored, though emerging area of interest on the materials landscape, due principally to their promising magnetic and catalytic properties. This review describes synthetic strategies for the formation of both supported and unsupported transition-metal phosphide nanoparticles, provides a summary of their relevant magnetic and catalytic properties, and indicates new directions for exploration.

4.
J Am Chem Soc ; 125(46): 13960-1, 2003 Nov 19.
Artículo en Inglés | MEDLINE | ID: mdl-14611223

RESUMEN

The reaction of Mn2(CO)10 with P(SiMe3)3 in coordinating solvents at T >/= 220 degrees C yields low polydispersity, highly crystalline MnP nanoparticles for the first time. The effect of dimensional limiting has resulted in the stabilization of a ferromagnetic ground state at low temperatures, rather than the metamagnetic state observed in bulk (microcrystalline) MnP. The synthetic methodology reported here is demonstrated to be general for a number of different metals and phosphine sources.

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